Startups usually don't have a ton of cash, so if you feel like you're still being shortchanged and the company simply can't afford to pay you more (from the company's perspective, increasing your salary may mean increasing everybody else's as well), you can ask for other things: more options, more days off, better benefits, and as you mentioned working remotely.
You're in a good position, and have built up good will over the years, so I'm sure they wouldn't want to lose you. It might be just a simple matter of bringing it up, so do that first.