These constitute my favorites. I can't narrow the list, because I deeply love each of these ... some for many years.)
1) THE BALLAD OF CABLE HOGUE (Goldsmith): "Tomorrow Is the Song I Sing"
2) UNA BREVE STAGIONE (Morricone): title song
3) DAVID AND BATHSHEBA (A. Newman): "The 23rd Psalm" end title
4) THE DOVE (Barry): "Sail the Summer Winds"
5) GOLDFINGER (Barry): title song
6) INTERLUDE (Delerue): title song (only on LP as far as I know, but Timi Yuro's album performance is superior to the film version)
7) LEGEND (Goldsmith): "My True Love's Eyes" (album version)

LILI (Kaper): "Hi-Lili, Hi-Lo"
9) THE LORD OF THE RINGS - THE TWO TOWERS (Shore): "Gollum's Song"
10) MONTE WALSH (Barry): "The Good Times Are Comin'" (Monte Alone)
11) PINOCCHIO (Harline): "When You Wish Upon a Star"
12) ROMEO AND JULIET (Rota): "What Is a Youth?" (Love Theme)
13) SEBASTIAN (Goldsmith): "Comes the Night" (both album and film versions, for different reasons)
14) TO SIR, WITH LOVE (London): title song
(What's with that smirk beside LILI above? I didn't put it there but also can't get it out.)