I have wanted a set like this since the first TOS trek albums came out. I think TOS's soundtracks are right up there with the iconic Star Wars soundtracks. TNG, DS9 and VOY... not so much. None of them had any memorable cues, except maybe for the episode Booby Trap and Inner Light.
I agree with you on DS9 and VOYAGER, but I'd argue that the first two seasons of TNG had pretty memorable music. It was around season 3 that the music got bland and forgettable for the most part.