There used to be tons of stuff exclusive to vinyl, but Randy is slowly narrowing that gap. Too bad I refuse to buy from iTunes...
Most of the stuff I needledrop are pop/rock albums that have superior mastering on vinyl than on CD. I do love playing with Disney Records, though, especially the mono records in the 3000 and 4000 series (ie, the semi-rare awesome ones). I'm still trying to find an original "Walt Disney Takes You To Disneyland," because the shiny new copy that came with the Musical History of Disneyland is TERRIBLE. The vinyl is dead quiet, but the master they pressed the record with is digital and has been HEAVILY no-noised - side two in particular is riddled with digital artifacts and "fish-tankiness." I'd really like to see how an original copy from the 50s stacks up against it.
Vintage Disney vinyl often sounds killer, though. I loooooove the Epcot soundtrack. The Official Album of Disneyland and WDW is about half and half, though - you can tell it was pulled from a variety of sources (most probably copy tapes) because certain tracks sound terrible while others sound fantastic.
Since I'm being a negative nelly (praising things just isn't as much fun), Ovation's "The Magical Music of Walt Disney" *looks* awesome because it has some rare material, but - as the liner notes state - almost everything is taken from the original 35mm film for the movies, NOT from the masters for the music itself. So what you get is what you hear in the films themselves - the music sounds medicore (movie film is NOT high fidelity, as the Fantasia soundtrack aptly proves), and it comes complete with dialog and sound effects to boot. Ugh. If I wanted something that sounded like this, I could just record my DVDs - and they'd probably sound BETTER.
You should also avoid the picture discs that were pressed in the 80s, unless you're just a hardcore collector. They were electronically processed from mono into "fake stereo" and sound terrible. God forbid they just leave it as mono - if it was mastered that way, leave it that way. Lots of mono recordings kick serious booty. If you really want the classic soundtracks on vinyl, the heavy duty originals in the 4000 series are the way to go, but they're rare and pretty expensive these days. Similar in quality but not QUITE as good are the repressings in the 1200 series. Flimsier jackets, flimsier vinyl, and sound quality farther removed from the master tape, but they still sound pretty darn good. Most of 'em, anyway. I've got a 1200-series "Peter Pan" that I bought sealed but plays incredibly noisy. Go figure.
Maybe I should just create a website for Disney vinyl reviews complete with comparisons to CDs. Might be fun... hmm. In any event, to end this post on a high note, I'm gonna give a shout out to two of my FAVORITE Disney vinyls, the ones I always end up spinning over again. First is the Adventureland Steel Drum Band. This guys friggin' rule and the record sounds awesome. Second is the Jazz Minors. They played in New Orleans Square in the late 70s and early 80s, and they sound exactly how you'd expect them to sound (which is a good thing). Sound quality on the record is great as well. I stumbled upon this one by accident while eBaying "Disneyland Band."
EDIT: I keep forgetting to mention something about needledrops - ClickRepair (http://wwwmaths.anu.edu.au/~briand/sound/software_download/clickrepair_info.html) should be in everyone's toolbox. It's the best click/pop remover I've ever used. Just keep it on relativly low settings (I have mine set to Declick 15 Decrackle 0) or it'll start dulling the highs and eating percussion hits. Avoid the other tools on that site though - No NoNoise is Good NoNoise.