The Force Unleashed

I'm not a gigantic fan of huge sets, but TFU was amazing. It introduced "unleashed" force powers and a bunch of characters with them. (Vader's Apprentice, ftw) Oh, and we finally got a FREAKING DARTH REVAN.

Champions of the Force

Wizards best all around set, I think. Added the Sith and OR factions, provided a boost in Force Users for the Republic and NR factions, and a force battery for the Rebels.

Knights of the Old Republic

Added to the Sith and OR factions with characters (some very misrepresented) from the KOTOR I and II games. The Mandos get some, too.

Legacy of the Force

This set and KOTOR were two great sets one right after the other. This one fleshes out characters from the Legacy books and comics: Cade Skywalker, Darth Caedus, Roan Fel, and Wolf Sazen among them.

Bounty Hunters

Introduced the game best shooter to date, Boba BH, and a crapload of Fringe characters. Also added the Mandalorian faction.

Universe

This is sort of a "meh" set. Thrawn, Lobot, Prince Xizor, Vader JH and Luke Jedi Master are all bright spots but there is also a bunch of pretty pointless characters: Nien Nunb, Dr. Evazan, Ponda Baba, the Kaminoan Ascetic and Nute Gunray.

Imperial Entanglements

I like it. The second 40 piece set enters some good Rebel commanders, a new bad-ass Vader, Palpy in his chair, and one of Mara Jade's aliases. Remakes include Thrawn, Dash Rendar, Lobot, and Xizor. Also a new R2, and the first completely useless piece C-3P0, Ewok Diety.

Clone Strike

Since I started with CotF, I don't have much experience with its predecessors. Clone Strike seemed like a good set though, with Aurra Sing and Zam Wesell for the Fringe, all sorts of Jedi (WITHOUT Double Attack) for the Republic and a bunch of useless tinnies for the Seps.

Rebel Storm

Since this is the first set, there was really nothing to compare it to. Solid pieces with generic abilities accurately portray the first three movies.

Revenge of the Sith

Solid I think, but kind of redundant after Clone Strike. Lots of remakes of Jedi , a very useful new R2, and some more not very useful Battle Droids.

Clone Wars

Based of the new movie, and the first of the new 40 piece sets. To me its seems very hastily done. The sculpting is not as detailed, and the stats are well on their way to making older sets obsolete (does EVERYBODY have Greater Mobile?). Bright spots are the new Grievous, who makes the Seps semi-playable, the new Aayla, the new Durge, and Captain Rex.

Alliance and Empire

Ugh. I know they were trying to commemorate the 30th anniversary, but the square bases and red cards were really a turn-off. It was a fairly balanced set though. I liked Quinlan, Infiltrator, Han in Stormie Armor, Luke CotF, the new Tarkin and Mara Jade, however. Oh, and Jawas!