I agree that might be nicely cathartic, but sadly, positive punishment-based behavioral modification a) has much less latency than other methods and b) has a really high chance of accidentally influencing the wrong behavior, since there’s no way to be precise about what the recipient associates with the external stimuli. So while you might be intending to discourage them from feeding wildlife, they might accidentally end up being less likely to engage with strangers, or just end up afraid of squirt bottles. (You have to keep in mind that whatever external punisher you might apply, like cold water, is probably going to have much less impact than the reinforcement of being close to / interacting with animals in that situation. The pleasantly reinforced feeding will outweigh the negative aspect of being bothered, and it will likely still occur again.)
One of the most successful ways of discouraging a behavior is when the punishing stimulus comes directly as a result of what the recipient is doing – so they’ll learn to change their behavior when they get bit, kicked, or scratched.
If you really feel like you need to contribute, you can try talking to them – or try contacting a park ranger or other appropriate authority to deal with the situation.