I tried this before, but the problem is, the reason many people/businesses have shitty websites is that they are not willing to spend money on it. I approached a few local shops (e.g. a comic book store) to create a cool website for them for a few hundred bucks, but they wanted it for free. If I would be a junior developer looking for stuff to my portfolio, sure. But I'm not, and not willing to work for free for anybody.
However, I might have given up too easily. I think I'll give this another shot