That is a difficult question because the songs vary in style so much that choosing some as better than others depends on the context of the song. I feel that many of the songs fit in with where they are placed in the films, but some of the cleanest, most effective use of songs, to me, include:
1) Bestest Friends (LBT 10)
2) Peaceful Valley (Wonderful opening song to LBT 2)
3) No One Has To Be Alone (LBT 9)
4) Beyond the Mysterious Beyond (LBT 7)
5) Always There (LBT 5)
These songs all protray important elements of the plot of each film, and show how the characters feel about what has happened very effectively. I would include "Very Important Creature" on this list if I had a 6th choice. If I had to choose some songs I felt could have sounded better, or could have been protrayed better for its purpose in the show, or for entertainment value, I would choose
1) Good Inside was one song which I have never values quite as much as the remaining LBT songs. The music wasn't especially interesting. They lyrics made sense, but they weren't anything spectacular. The song seemed slightly out-of-place, though not terribly. I simply never found "Good Inside" to be one of my favorite songs to listen to, for the purpose of listening to it. It just never appealed to me.
My personal favorite songs to listen to, for the sake of listening to songs depends on my mood, however some general choices include
1) Beyond the Mysterious Beyond (I love the LBT 7 end credits version
)
2) Peaceful Valley
3) Adventuring
4) Bestest Friends
5) Family
I must add though, that there are a number of other songs I would include on these lists if we could choose more. This is a difficult question, as many of the songs suit their purpose very well, and many of them are interesting to listen to.