I'd pick GTA(the original) probably as it was great, it complimented the game very well and very humourous. I could also choose the rest of the series with the exception of GTA2 and GTA London but it is cheating slightly I think because they are using songs that have been released commercially, not simply songs that were written solely for the game.
K I am a massive fan of PC games but my fav soundtrack from any game has to be 'RED DEAD REVOLVER' on PS2 lol I loved everything about that game. It is a rockstar game and of course like most on this thread I loved the gta3 and vice city soundtracks too.
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