I know I shouldn't admit this, but the Electric Dreams soundtrack is one of my favorites to this day. (And I've never seen the movie, nor do I want to.)

totally cheesy and waaay out of my demographic, but I have a real soft spot for the Sleepless in Seattle soundtrack. Nat King Cole, Jimmy Durante, Louis Armstrong, Tammy Wynette, Gene Autry, Carly Simon. a great collection of classics with only one real 90's contemporary dud courtesy of Celine Dion.

I like Cliff Martinez' scores for Solaris, and to a lesser extent Traffic. Cooled-out cinematic emotional ambience.

other favorites: Pulp Fiction, The Life Aquatic (and Rushmore, for that matter), Good Morning Vietnam, The Graduate, Harold & Maude.

The work Billy Corgan did on Ransom is my single all-time favorite OST. YMMV.

Bump bee ba ba. Bump bee baa baa ba ba.
*I did it for you*

The Donnie Darko sound track is great, and despite what it says about me (I don't like music from the '80's - really), I'd also love to get a copy of the soundtrack from Grosse Point Blank.

The soundtrack to Until the End of the World is excellent (and well known for it). Lots of big names, but enough material that slipped most people's notice. The film isn't so great, but the music makes up for a lot.

And then there's Velvet Goldmine. Again, most of it isn't obscure, but worth listening to for songs written for the film alone.

I still love portions of the Xanadu soundtrack. I also really like The Life Aquatic and Royal Tenenbaums. Oh, I enjoy the Broken Flowers soundtrack quite a bit too.

Polanski’s The Ninth Gate was a mediocre movie, but I loved the moody classical soundtrack.

I like Howard Shore's work for Cronenberg, and Angelo Badalamenti's work for Lynch. In particular, Naked Lunch and Crash for the former and Twin Peaks, Mulholland Dr for the latter.

For soundtracks that are compilations of popular songs, I'm fond of the Crooklyn soundtrack. For more recent soundtracks that are a mix of pop and compositions scored specifically for the films, I like the already mentioned Mothersbaugh / Anderson: Royal Tenenbaums. (Rushmore ain't bad either. Haven't picked up Life Aquatic yet).

The first I ever bought was the Vangelis crafted Blade Runner soundtrack and it's still one of my favorites. Shortly thereafter, I picked up the Akira soundtrack which is also good times. I think I'm going to put that one on now.

the soundtrack to koyaanisqatsi served as my introduction to philip glass, and it's still my favorite work of his.

before seeing vanilla sky i'd never heard of sigur ros. plus, it has that alternate version of "have you forgotten" by red house painters and that cool little cheesy techno song by looper that xerox still uses in their commercials...

Carter Burwell does some great stuff. He does all the Cohen Brother's soundtracks plus many more. His first score, for Blood Simple, has one particularly beautiful theme in it. (Full disclosure, we were house mates for many years.)

Malkovich Malkovich

I forgot last night the very first soundtrack I fell in love with: it's for the movie Touch (possibly Skeet Ulrich's finest moment as an actor, in a Christ character role) and composed by Dave Grohl. the music is a step away from anything else he's done musically, sort of surf rock psychedelia for the late 90's.

syntax: I'm always excited when a new Cameron Crowe movie comes out, just for the soundtrack. the Vanilla Sky ost is great, and I had a similar experience to yours on the Jerry Maguire soundtrack (of all movies, sheesh). I'd never heard of His Name Is Alive before listening to that movie.

Repo Man is a classic, of course. Pump Up the Volume is another good shouty soundtrack--the Rollins/Bad Brains version of 'Kick out the Jams' alone is worth the price of admission, IMHO. I'm also very partial to the City of Lost Children soundtrack, though I still haven't replaced it after a roommate stole it a while back. The soundtrack to Latcho Drom I would've stolen from a (different) roommate, if I were a different sort of person. Such gorgeous, energetic music.

Here are a few favorites in no particular order:

Together Brothers - Barry White/Love Unlimited Orchestra
Coffy - Roy Ayres
Made in U.S.A. - Sonic Youth
L'Ascenseur pour L'Echafaud - Miles Davis
Anatomy of a Murder - Duke Ellington
Touch of Evil - Henry Mancini
Odds Against Tomorrow - Modern Jazz Quartet
Trouble Man - Marvin Gaye

Also, I'd like to second Philip Glass' work on the qatsi movies, and plug Ennio Morricone's spaghetti western scores and John Zorn's Filmworks series (ooh, also The Big Gundown, come to think of it)--there are something like twenty volumes now, and I think that, collectively, they're among his best work.