I don't think there were a lot of PC games with a *commercial* (separate / retail) OST release that are now hard-to-find or super-rare. Most of them were bundled in with the game.
The recent revelations that there were soundtrack releases in certain retail stores / regions for the Elder Scrolls games Daggerfall (II), Battlespire (a side-story), and Redguard (another side-story) ... that's probably some of the rarest PC music I know about. The two "Origin" discs are super-rare as well.
I guess there are Japanese PC games which got OST releases which are now rare / OOP. Plenty of Falcom games probably fit that category, if you exclude their digital release. ... Ys Origin OST is the first that comes to mind.
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