I tend to avoid companies with "unlimited vacation" because their employees seem to take even less vacation than they would have otherwise, don't get compensated for it as a result when they leave, and feel pressured to not take it in the first place. (See https://news.ycombinator.com/item?id=7613526 and many other stories.) It's even worse when the bosses present a terrible work-life balance to employees.
I basically think back to one of the times I've been really sick but not contagious, or my honeymoon, to figure out if I like a vacation policy or not. Minus 1-2x/year for crunch times, assuming I'm keeping up with my workload, would I have taken a day off? Would I have felt like I couldn't take the time off? Would people have been receptive to me working from home? Now double that time off if I want to have kids in the future, am I still okay with it? Sad to say many unlimited policies don't make me feel comfortable on any front here.
What happens if an employee falls on stairs and spends the next two months in hospital and then another one in bed, at home? (happened to a colleague of mine)