Contact - There's a few commentaries on the version I have but the good is with the special effects guys. They give a fascinating account of all the SFX in the movie, 90% of which you wouldn't even know was there!
Dark City - Roger Ebert gives a fascinating running essay on the film. Great if you're into film theory.
They're the 2 which come immediately to mind. I must confess that I don't tend to listen to commentaries these days as most of them are pretty dull so I really need a good reason to switch them on.
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