I'm a bit of a soundtrack junkie, so I have quite a few in my collection. In terms of my favorites, I'll narrow it down to these:
Batman Begins: I also own the OST of The Dark Knight, but I enjoy Batman Begins a little more. Both soundtracks do well to emphasize the dark and more gritty revamp of the Batman franchise, but the themes in Batman Begins seem composed better and are more memorable to me.
Edward Scissorhands: Hunted this down mainly for the song playing at the end of the movie and Ice Dance. While those two songs (and a few others) are sweetly sad, there's still some songs that have Danny Elfman's quirkiness to them. This OST has a nice mix of that throughout. ^^
Sweeney Todd - The Demon Barber of Fleet Street: I have the OST from the movie, and a few songs from the broadway play. I enjoyed the dark lyrical content of the songs.
I have a few Disney Soundtracks from the animated movies, mostly because they're damn catchy. My favorites would probably be Beauty and the Beast and Tarzan. The Tarzan soundtrack is fun and really catchy (and features music from Phil Collins~), and the OST of Beauty and the Beast is just wonderful, particularly Be Our Guest.
Pirates of the Caribbean: Dead Man's Chest - I used to have all three soundtracks from the three movies, but they started to sound a bit samey to me, so I downsized to just a few songs from the second film. Love the jauntiness of some of the tunes.
Prince of Egypt - Picked this up because I wanted The Plagues and a few of the orchestral works, but the whole OST is pretty powerful, and very fitting of the subject matter of the film.
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