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My favorite set would be Warlock Tier 6 (Malefic Raiment), and it would be worn by a Gnome, it just screams "Hey! I'm a tiny master of doom!"
I personally think the TBC Dungeon set for Rogues, Assassination Armor (Assassination Armor), is the coolest looking set in the game. Of course Paladin T2 or Warlock T5 or Priest T6 are all stellar, but the simplicity of Assassination Armor makes it my favorite tier set.
The paladin's judgement set was obviously the best. After 60 levels of hearing "retlol" it was finally time to kick some ass. Add to the fact that it was the best looking thing anyone had ever seen at the time :).
Easily Shaman tier 5, the Cataclysm set. Not only did the physical dps set give us a sort of maelstrom weapon effect with healing surge, it also looked especially intimidating with the matching Claw and Fist of Molten Fury. A shame that the fist had a 1.5 speed which made it completely useless for any Enhancement Shaman worth their salt, but hey, at least it looked pretty!
Dreadnaught's Battlegear is my favorite. It just has a certain sense of simplicity, and at the same time has a sense of strength. Plus the shoulders are badass.
I loved the original vanilla Teir 2 sets mainly because most of them really looked like the class.I mean you saw stuff that you could expect to see on most of the classes such as the famous Paladin Teir 2: Judgement.They put really good coloring and good design into the older sets for what was probably known as the most famous Teir.
Vestments of Faith was the best tier set. even though tier 7 had the same halo and wing effect, the light blue and white coloring on tier 3 fits a healing priest more than the re-colors do. it's really too bad that blizzard made it unobtainable now.
Tier 2 Paladin armor set - Judgment ArmorNothing seems to really iconify paladins more than this set.
I loved the shaman Tier 8 shoulders and helm. They seem to fit the class and have a great look