They all have really good qualities, but I'd still say I cared less about San Andreas and 3. I didn't play the PSP ones and I don't really want to 'cause they don't seem significant. Vice City is the best probably while GTA4 is a very very close second since the gameplay is the best.
It's a toss up between San Andreas and Vice City. Vice City for the soundtrack, and San Andreas for no load screens and the ability to steal a plane and just fly around, parachute out, repeat.
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