This is one thing I never understood, especially when people try to use them for small purchases. At my workplace, the store owner has disallowed us from accepting $50 and $100 bills in order to avoid having to check for counterfeits. People get very upset at this policy.
One time, a customer came up to the counter with the items they had picked out. I scanned them all up and then provided her with the total. She then tossed a $50 bill on the counter. I politely explained that due to store policy, I would be unable to accept it, so she'd have to either break the bill elsewhere, or she'd have to provide a different payment method.
In response, she snatched the bill off the counter and angrily said, "Well, I'm never shopping here again." She said this loudly enough that it took aback multiple nearby customers, who began to look on.
After digging in her purse, she tossed two smaller bills onto the counter, which turned out to not be enough to pay for the total (after the cash she still owed $7-8). I explained this to her, and then she snatched the cash off the counter and left. The next customer I interacted with, who had witnessed everything, told me that she'd "go easy on me". Haha.
I understand it can be frustrating to not be able to pay with the money you have on you in the moment, but I wish customers would understand that the store owner sets the policies, not the people working for the owner. Retail workers don't really have any power in that regard, we just work here. Also, I wish they'd understand we are not a bank; even if we did take larger bills, we don't have a million dollars in the register to give you. Usually, we have just enough to get through the week. It's just a nuisance.
Didn't seem like this customer was thinking you had any power here. I'd probably do the same thing and just walk away and not return rather than go on another errand so that I can spend money at this specific store. Walking away rather than trying to argue it implies they didn't think there was any point in arguing (or didn't think it was their place even if they thought they could get something out of it).