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+1 for Black Lagoon, W anime pick.
Also for Ghost in the Shell, PatLabor, and Redline.
I will also add on:
Jin-Roh/Jin-Rou (not the Korean live action from 2019), but it does briefly show a child on screen as a supporting character, and I dont remember if Kei was over 18-20 or not
AD Police Files, and its related series Parasite Dolls (unfortunately, the other related series Bubblegum Crisis and Bubblegum Crash are disqualified because Nene Romanov is 18 and Priss is 19, both under 20)
Space Dandy (maybe, that anime had like a billion characters and I dont remember if all of them were adults or not, but its not exactly a kid oriented anime)
Black Lagoon is one of the most underrated shows. People who have seen it usually love it, but not enough people have seen it.
I need to watch Jin-Roh sometime.
Yeah, Black Lagoon is lots of fun. I was so sad that it ended.
Jin-Roh slaps, just make sure you're prepared for it. It's a pretty heavy, typical Japanese war film, I don't want to spoil anything so I will just leave it at that. Soundtrack is god-tier though.
Patlabor 2 is one of my all-time favorites, but it's not very well-known. In a way it feels too mature and slow to be a wide hit, I guess.
Mushishi. Very serious, well-told stories told in single episodes. Occasionally a younger character will come along, but it's mostly adults, and the cast outside of the MC rotates episode to episode.
In no particular order these come to mind. Most of these are outside what I typically watch, but I did enjoy them.
Monster (Crime Drama) https://anilist.co/anime/19/Monster/
Mushishi (Psychological Slice of Life) https://anilist.co/anime/457/Mushishi/
One Punch Man (Comedy Action) https://anilist.co/anime/21087/One-Punch-Man/
TRIGUN (Action Adventure) https://anilist.co/anime/6/TRIGUN/
Hellsing (Vampire Action) https://anilist.co/anime/270/HELLSING/
Overlord (Evil Fantasy) https://anilist.co/anime/20832/Overlord/
I think a lot of the other answers here are being too generous with your rules and not giving you characters that both look older and are older.
I've completed quite a few:
Honorable mentions - depends on how strictly you'd define "mostly":
Honorable mentions - unique circumstances:
The only one I'd take issue with here is Spy X Family. I think it's more of an "all ages" show that focuses heavily on Anya and her classmates antics. All the rest make sense!
Oh yeah, her classmates. They are so unmemorable that I forgot about them😅
Moving it down to honorable mention
Ghost in the shell stand alone complex (and 2nd gig) was my first and still favourite anime.
My favorites have been :
Redline is unironically one of my favorite movies. It's just so silly, and I love it. "We're losing the race, what do we do!?" "What if we pressed the pedal down...harder" And then they go faster.
Welcome to NHK, really walks you through the life of a university dropout failed adult.
I loved Wotakoi. The 4 main characters are 26-28 and employed. It's in the especially rare category of adult romcoms. It's a shame the anime never got a second season, but the manga is finished so if you give it a watch and want to find out what happened after, give it a read!
Wotakoi is basically my default answer to when people ask about adult romcom series. Great suggestion.
Big O
Ninja Scroll
Read or Die
Samurai Champloo
Berserk (OG)
Blue Gender
New:
Old:
Other:
Frieren - Beyond journeys end
A real fresh take on fantasy stories imo with a lot of themes I always wanted to be explored in the genre. In my last pen & paper group i played an elvish alchemist specializing in seemingly useless utility potion effects. And when i created the character i had a hard discussion with my dm on how elves actually pervice the world and other races, with them reaching ages of thousands of years and whatnot. And frieren adresses that perfectly. Also that soundtrack is just the best. I have yet to listen to "One last adventure" and not get at leas queazy, if not tearing up a bit.
Were currently watching it a second time, just a week after finishing first time. We've never done that with any series.
Highly recommended
Fern and Stark are technically in the 18-20 age range though. And fairly teenage-y. But I agree it does explore a lot of more "mature" themes.
Odd Taxi (crime drama)
Psychopass (crime drama)
Cells at Work: Code Black (... Medical drama?)
Death Parade (Death game-ish)
Devilman Crybaby (main character is a high schooler, but it's irrelevant imo. I didn't remember until I looked it up again. This is a grim series )
Inuyashiki (Action. Old man is a complete Chad)
Panty & Stocking (Comedy)
Jellyfish Princess (Drama)
Saga of Tanya the Terrible (it's not really a kid, action)
Saint Young Men (Comedy)
Samurai Champloo (Action)
Shiki (Horror/Drama)
Monster (Mystery)
Rose of Versailles (Very old, but romance/drama)
Almost all of Satoshi Kon's work (including Paranoia Agent)
Ruroni Kenshin (Shounen)
Yurii on Ice (Romance/drama)
This was harder to answer than I thought, pushing up to 20 eliminates a lot of contenders I think. I would say maybe Vinland Saga? The main character starts as a child, but it also covers a large time span so he hits twenty partway through the second season. Major recurring characters are almost all adults throughout. Its a semi-historical anime set mostly in England and Denmark during a war between the two. It's a show that deals heavily with violence and trauma, has some very complex characters, and I can't recommend it strongly enough
Eureka Seven
if you want a fantasy story with emotionally intelligent characters, well-crafted themes and messages, great animation and music
this is a gift for you
OP2 Spoliers
Eureka Seven Opening 2 HD High definition
A few off the top of my head: Shirobako. Space Dandy. Samurai Champloo. Ghost in the Shell: SAC.
Loving all of the Odd Taxi mentions.
From my spouse:
Not sure if it's considered true anime, but Castlevania on Netflix was excellent.
The recent film Blue Giant is great. About a young man who moves to Tokyo from rural Japan to pursue his love of jazz. Great visuals and music.
Genshiken
Bartender
Spice and Wolf
The Fable
Dungeon Meshi
Goblin Slayer
Saihate no Paladin
Shirobako
Psycho Pass
Wotakoi
Zom100
Golden Kamuy
My Home Hero
Kyokou Suiri
Vinland Saga - He's like 16 in the first half but grows up by the 2nd half.
Isekai Ojisan
Cyberpunk: Edgerunners
Blue Period
Megalo Box
Samurai Champloo
BNA
Aria
Ishuzoku Reviewers
NHK no Youkoso
Drifters
Trigun
Osomatsu-san
A lot of people already mentioned the ones I know of and mostly I only know of older shows that were geared to an older audience :/
Outlaw Star? Anything made by Satoshi Kon texhnolyze Megalo Box Baccano? Legend of The Galactic Heroes
Wotakoi, Black Lagoon, Baccano (I think?), 91 Days, Akudama Drive, Golden Kamuy, Hakata Tonkotsu Ramens, ID: Invaded, Dragon Maid, Spice and Wolf, Wave Listen To Me! to name a couple
(trying not to duplicate other mentions)
Current:
Recent:
I'd tentatively add Berserk to the list. Tentatively because the story does go back to recount the characters' youths, but that's really not the main focus.
Another good one with mostly adult cast and a more mature plot is Monster.
Off the top of my head, Darker than Black. Same director, different take on bleakness: Wolf's Rain. The main characters don't really have 'ages' given, but they're pretty clearly adults.
Record of the Lodoss War (a D&D campaign turned into anime, if I recall rightly)
That time I reincarnated as a slime (technically the main character is ~34, and very few children are shown, but the cast has a lot of 'childishness' in them... the style is the equivalent of a popcorn superhero movie I'd say)
Legend of the galactic heroes
Witch Hunter Robin
Van Helsing (if you just want to laugh at idiocy, simply watch the abridged series, but the actual show is good)
Dragon Ball Z, except for a few episodes every now and then. The show itself is obviously aimed at the younger shonen crowd though, if you haven't seen it.
.hack//sign (dot hack sign) is a pretty interesting one. It has several other series in its 'canon' if you like it. I'd say it was the adult oriented, well-presented premise of sword art online before sword art online was wet-dreamed up. A friend described it as 'waving its dick around because they had an actual orchestra for the soundtrack' in several scenes.
Shirobako
A Sign of Affection
Showa Genroku Rakugo Shinju
Call me a bit old fashioned, but Lupin III. Regardless of which part or movie, I tend to enjoy some of the sometimes wacky antics that occur.
Lots of good stuff in this thread already, will suggest Black Magic M-66 and Megalobox.
A few older series I haven't seen listed yet:
Heh, does western anime count?
Legend of Korra, Vox Machina, DOTA: Dragons Blood
And Pantheon.
For heaven's sake, if you have not watched Pantheon, correct that immediately. Techically the cast is young, at first, but it doesn't feel like that at all.
The new Bartender anime was pretty good.
Vinland saga
The Great Passage and Showa Genroku Rakugo Shinju. The latter of which might start with them as kids but I feel like most of the show was with them being older.
"The Saint's Magic Power is Omnipotent" was pretty good. I agree with lots of the others people already listed, but this one makes her age a relevant plot issue which basically sets the tone. It's a romance anime with light combat and a good amount of world building. 2 seasons.
Golden Kamuy comes to mind.