I'm going for:
1- Moblins (The Wind Waker): when they capture you in the Forsaken Fortress, ceaselessly block your sword attacks (looking infuriatingly smug at the same time) and send you flying with their spear swipes and punches, it really makes me want to smash their stupid, ugly faces in!
2- Fire & Ice Keese (Ocarina of Time): it is disconcerting when they dive towards you, but burning/freezing you on contact is even worse, and they FLY AWAY before you can punish them! This makes me prefer the later versions of Keese in The Wind Waker and Twilight Princess, who kindly let you kill them before they attack.
Despite freaking me out with their moans and screams, I quite like the Re-Deads.