No. I do notice some of the games that have bad screen tear or poor fps, i.e. Mass Effect, as mentioned. However I buy most of my games on the 360 by preference - incluing FO3, Bioshock, Far Cry 2 etc. I just prefer the large screen, ease of playing etc. that can be had on a 360/PS3. Also some of the XBLA downloads have been essential; i.e. Rez & Ikaruga reworkings.
My PC then gets used for MMO's or PC only games (i.e. Kings Bounty), or older PC Games (Diablo 2 or Baldur's), or essential MP fun (like TF2).
That's the way it's panned out this generation for me. I guess I've always prefered owning console games, and the difference on titles to date hasn't given me much to think about. Something like Dragon Age, could be tricky where if I buy I'm again leaning towards the 360 version.