A good GM should should try to involve multiple avenues to involve the players in the game. Music is one of those avenues. Now, the first place I would go for recommendations is the Soundtrack Saturday series at The Word of Stelios. Other than what has already been posted there, here are some of my recommendations:
– Any soundtrack from an Infinity Engine game (Baldur’s Gate, Baldur’s Gate II, Icewind Dale, Icewind Dale II, & Planescape: Torment
– Endless Legend
– Arcanum: Of Steamworks and Magick Obscura
– Any soundtrack from The Elder Scrolls games (particularly Morrowind & Skyrim)
– Dragon Age: Origins
I know that these are videogame soundtracks, but I find that they are designed to be background music during particular gameplay segments. By mixing and matching the appropriate tracks, you can create exactly the mood need and, if you create a few playlists, you can quickly adapt to what is happening at the table.
Exploring a creepy dungeon? Queue up “Creepy Dungeon” playlist. Ambushed by a seven-legged monstrosity from beyond the stars? Bring up the “Fightin’ Time” playlist. Celebrating a successful battle at the local taven? “Tavern” playlist time.
Making a tabletop experience more multimedia will make it more memorable. Just don’t be too loud!