Those would be the top two considerations for me, personally. Nothing against the rest of his catalogue in any way shape, or form (he's one of my top emcees - I love 'em all!), but Labor Days and The Impossible Kid are both pretty pinnacle points at different ends of his career. Sure Skelethon really brought forth the new flow, but the sudden emergence of personal introspection that came with The Impossible Kid is an undeniable paradigm shift for him - and he rocked it well.
Hell, Bushwick would have been a more inspired choice than None Shall Pass, although very left-field and a bit daring since it's an instrumental film score. Or, as I mentioned in the past, finally reissuing Music for Earthworms would have been a monumental coup. Otherwise his solo stuff is all, thankfully, very readily available.
Now Hail Mary Mallon or The Uncluded... those would also be some very daring and exciting choices!