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The Malefic Raiment set (Warlock Tier 6) will always be my personal favorite. Just look at those demon wings! Absolutely magnificent.
The Druid's tier 6 aka Thunderheart armor was the best tier ever created. =) http://www.wowhead.com/itemset=678#screenshots:id=56659 It suits the Druid class so beautifully and lets face it, every Druid's wet dream is to look like Hamuul Runetotem xD
The best set is the Field Marshal's Battlegear...espcially when a paladin is wearing it.It just fits a paladin so well.Also in vanilla when you saw someone in a battleground in that gear, you knew you had to run or you would get your ass kicked.
I love the Warlock tier 4, Voidheart, simply because it was the first tier set I was able to get and complete. The stats were not that great, it wasn't all that great looking but it was mine. By the time I had all the pieces we were progressing in Serpentshrince Cavern and Tempest Keep but I still had the entire set sitting in my bank.
I'm not sure my answer will qualify, because I started playing in November. But I like the current tier set (well, except the name for the rogue's set... WIND DANCER! Seriously!)
It's honestly a toss up between:Paladin tier 2 - JudgementWarlock tier 10 - Dark CovenWarlock season 1 (tier 4 re-color) - Gladiator's / Voidheart
Ymirjar Lord's Battlegear the warrior T10 set. It was the first full set of armor I obtained on my main character with my first experience of end-game content at level. It looks amazing on a dwarf as well.
Warlock tier 8 is my favorite whole set to wear; it's the only one I went back for to get all the pieces with surplus higher tokens. I'm not a fan of t6 color scheme, so this one represents the warlock class in atmosphere and story to me. Putress was a perfect candidate for role model, especially as affliction; he's out to make the world suffer their way to the afterlife rather than swift spells of killing (fire has some symbolism of rebirth; plague and afflictions of the body are just slow death). It's consciously evil, which is quite delicious when you love well-played villains like I do.(The only other tier that's appealed aesthetically to me has been the Voidheart Raiment (t4), and that's more because with that helm showing, I have a sudden urge to stand on top of people and give them big ninja hugs.)
Rogue T2! (The redone version)It just looks beautiful.
My favorite set is still the Tier 2 Paladin set known simply as JUDGEMENT ARMORJudgement just had the perfect mix of bad-assery and class specific flavorperfect example of this is are the shoulders which shows an open spell book with a sword. Also over all it appeared to be priest robes mixed with plate armor.People often bring up the idea of having an appearance tab where you can pick which armor shows.... Judgement is and will always be my reason for doing this!sorry I tried to link it within the text but I couldn't figure it out, lol Judgment Armor