I remember there was this one time back in the '80s where I put together my own version of a tracked ST episode score by recording different cues from the various LPs onto my cassette deck -- not trying to replicate an existing tracked episode score, but trying to concoct one of my own for a hypothetical episode. I don't think I had any specific story or scenes in mind; I was just trying to convey the impression of a story progression, experimenting with the process of how a music editor might create a tracked score. (I don't have the tape anymore, however.)
I suppose with this set, one could do that same kind of creative exercise much more authentically, since you'd have the same full repertoire of original tracks that TOS's music editors would've had to work with. Maybe one could assemble playlists to accompany one's TOS novels or comics.
However, I think my personal preference now is just to hear the cues and scores as they were originally written, and not mix and match different composers, different themes. Heck, it was my preference then; my experiment was as much about exploring the process as hearing the result. And these days, with modern tools for constructing "playlists," the process would just be too easy to interest me much.
Sounds like great fun, and reminds me of projects I did with the first home computers, painting images one pixel at a time to reproduce iconic Trek images. Hopefully someone will have fun with this set in much the same way as we did.