To echo Sierra1, I have used both and I think either are decent options, but Plasti Dip in the rattle can is by far the easiest. Goes on easy, peels off clean. Vinyl is tricky to work with and doesn't come off as easy as Plasti Dip, but it is more durable than Plasti Dip (or at least can be if you use pro grade).
If you have curves, bumps, etc. then vinyl can be a pain to work with. Go slow, use heat, be careful. Plasti Dip goes on easy and can be built up to hide imperfections. If I can find some pictures of one of my old dipped bikes I'll post it for reference.
Update: this is the only picture I could find. I've Plasti Dipped a whole bike before, but this picture is only of the forks
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