I love TNG but I've seen them all a million times. I've seen most of TOS, most of DS9, probably half of VOY, never seen ENT.
Just got done watching VOY S7 E5 "Critical Care" and thought it was pretty good ("The Doctor is kidnapped from Voyager by an alien who sells him and his mobile emitter to a hospital hovering above a densely populated planet").
My all-time favorites are from Next Generation: "Darmok," "Lower Decks," "The Inner Light," "The Best of Both Worlds," "Unification," and "Data's Day"