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This is one task I have never tried, I am wondering what forum readers would count. I am not interested in unique items (daedric artifacts, dragon priest masks etc.) but complete sets that are not part of the regular Smithing skills. Obvious ones are Thieves's Guild, Dark Brotherhood, Nightingales, Archmage (okay not a complete set), Dawnguard and Miraak. Others I probably don't count as they are variations on one of these, various combinations for Dark Brotherhood, Guildmaster, Linwe's armor.

So, any others I should get to complete my collection?
 

Lady Redpool the Unlifer

Pyro, Spirits Connoisseur, and Soulless Anarchist
There's a second variant of elven armor(elven light, gilded?) that you can't craft.

Though it's clothes rather than armor, there are the jester's outfit pieces(not cicero's)

Stormcloack and Imperial gear

Forsworn armor.

That's all I can come up with right now, I'll add more if I think of any.
 
Thanks. I also remembered Dawnguard and Vampire. I will not include all the different town guard outfits. Got to start building those mannequins!
 
I can't help but do this!

My general modus operani is to keep one set of each standard armour, and generally ignore any enchanted variants that are found/given as quest rewards. Then I go after the genuinely unique bits. They don't even have to be full sets though, like the Ebony Mail for example, just unique. So things like the Targe of the Blooded are fair game.

As for the (mostly) full sets, in addition to what's already been mentioned above, I know of:
  • Wolf Amour - Granted, not quite a full set, but close enough for the purposes of a mannequin.
  • Penitus Oculatus armor - You'll get more sets of this than you know what to do with if you play through the Dark Brotherhood quests, but if you don't, they have an outpost in Dragon's Bridge, if you fancy committing a felony to get a set.
  • Miraak Cultist 'armour' - This is a mixture of light armour and clothing, but I still count it as a set personally. Plentiful, as Bethesda thinks that the best way to encourage people to play the DLC is to constantly annoy them, apparently.
  • Stormcloak Officer Armour - If you're not following the Civil War questline, you can get a set by finishing the Dragon Cult quest in Forelhost.
  • Ulfric Stormcloak's armor - You will, of course, need to murder Skryim's truest hero to get it.
  • Morag Tong armour - I think this was added in Dragonborn. If memory serves (I haven't played through DB as much as the rest of the game), you get these as part of the quest that sees you investigating the ash spawn problem for the captain of the guard in Raven Rock.
  • Skaal armour - Speaking of Dragonborn, the Skaal have unique armour too. I think you can find a couple of sets lying around, though I don't remember where. But if you see some hunters, and watch if they get killed by a Netch...
  • Ancient Falmer armour - You get this near the end of the Dawnguard questline.
  • Armour of the Old Gods - I tend to keep this instead of keeping a set of regular Forsworn armour. You can get it during the Escape from Cidna Mine quest, depending on who you side with (guess who you'll need to side with!). It is just a normal set of Forsworn armour with enchantments, though.
  • Falmer Armour, and Falmer Hardened Armour - While they're quite common underground, they're not seen much outside of Falmer infested areas, and you can't craft them, so I count them as unique. The normal, light, pre-DLC version is difficult to find in its entirety - but I think you can get a complete set in the same ruins as where you find Mjoll's sword though. Don't wear it in cold areas if you're a female, though. It's, erm, it's not exactly warm.
  • Ancient Shrouded Armour - It may look identical to the regular set, but it's vastly superior, and it's ancient, so I consider it collectible for that reason alone! YMMV, of course.
  • General Tullius' armour - You will, of course, need to murder Skyrim's one true hope to get it.
I'll check my chests when I get back home (in real life and in Skyrim) to see if there are any others.

EDIT: Oh, there's also...
  • Fur armour - You can't craft it, so it technically counts as unique I guess?

There's a second variant of elven armor(elven light, gilded?) that you can't craft.

It's the light variant you can't craft. They're easy enough to find though, as it seems to be the standard uniform for the Thalmor soldiers.
 
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Need I remind you of the Ancient Nord Armor? The Helm Of Yngol is another one. The shield of Solitude. The Shield of Ysgamor. There are also unique forms of mage robes. The Forgemaster's Fingers. Nozer's Helm.* The Helm of Winterhold.* *These are found for specific quests in cities. Valmera Priest robes. Mystic Dawn Robes. In addition to unique armor pieces, there are also unique weapons.
Here are some I know of:
  • Blade of Sacrifice
  • Blade of Woe
  • Blade of Hjaalmarch
  • Axe of Windhelm
  • Axe of Whiterun
  • Ebony Blade
  • Nettlebane
  • Several Unique Mage Staffs
  • Valider's Lucky Dagger
  • Kavoen's Dagger
  • Dragon Priest Dagger
  • Scimitar
  • Chillrend
  • Grimsever
  • Wuuthand
  • Dawnguard War Axe
  • DawnGuard Warhammer
  • Harkon's Sword
  • Blade of the Pale
  • The Pale Blade
  • Ghost Blade
  • The Imperial Weapons
  • Auriel's Bow
  • Nightingale Blade
  • Nightingale Bow
  • Mehrunes's Razor
  • DawnBreaker
  • Red Eagle's Bane
  • Red Eagle's Fury
  • Drainheart Axe
  • DrainHeart Sword
  • Drainheart Battleaxe
  • Ancient Nord Sword
  • Ancient Nord War axe
  • Ancient Nord Battleaxe
  • Ancient Nord GreatSword
  • Ancient Nord Bow
  • All the Unique Arrows
  • Crossbow
  • Blade of Falkreath
  • Blade of the Rift
  • Blade of the Reach
  • Lunar Iron Sword
  • Lunar Iron War Axe
  • Lunar Iron Mace
 

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