"Best?" I'm not sure I can tell. The Freelance Astronauts are typically pretty entertaining, even if Maxwell Adams is terrible at Zelda games (at least, the two that I watched). AccountingNightmare (who's work I'm currently on) is pleasant to listen to and genuinely good at the Devil May Cry games, though she goes the more informative route than entertaining (letting the games speak for themselves in that regard, I think). Kung Fu Jesus and Thuryl seemed to go for both in their God Hand and Might & Magic 2 (respectively) LPs. And listening to those guys who did Kaizo Mario World was schadenfreudtastically funny.
I haven't tried Spoony's stuff yet. Still, of the other TGWTG affiliates I love Linkara's LP of Star Trek: Elite Force, and Paw's LP of King's Quest 5 essentially got me into the art, so I'll check him out.