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I'll be applying for Fall 2015, and I have one professor who agreed immediately to write an LOR when I asked a few months ago, and another who still has yet to respond. I've emailed him 3 times, in April, May, and a few days ago. I would go in person to ask, but I went to school in Illinois, and I currently live in Georgia. I feel like I had a good relationship with this professor (I was a research assistant on two of his studies, and he offered to be a reference when I graduated two years ago). I'm getting a little nervous since he's the type of person who's always on his email, and I'm sure he must have seen at least one of my messages. Should I take his non response as a no?

You should at least start looking for another rec if nothing else. You should be looking for another rec regardless since you already have a college prof rec and you're 2 years out. Softs don't matter much but it might look a little suspect if you don't have any recent rec's and you're on the borderline/WL pile.

No, if you're only 2 years out prof letters are perfectly fine. I would try calling his department to get his office number/office hours and call during his office hours. He may have been on leave or something - some profs ignore student e-mails while on leave.