Except for Munch's Oddysee (yet another design flaw of MO was the music, IMO - Didn't add atmosphere to the game at all), pretty much all of the music from the Oddworld games is quite awesome.
Still, it's hard to decide. For me it's a tie between AO and SW. Abe's Oddysee's score was a strong part of the atmosphere for all the levels, especially Scrabania and Stockyards. Stranger's score fitted well to its game too as well as sounding really amazing in most parts, but I get the feeling that it wasn't really an integral part of the game's atmosphere somehow.
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