Ocarina of Time no doubt. First he visits you in your nightmares. Next, he curses the Great Deku tree. Then, he puts the Gorons into a famine. Then he attacks Hyrule Castle and causes Princess Zelda to flee. Then, he laughs at you for taking the Master Sword, which opened the way into the Sacred Realm, where he obtained the triforce of power. Next, he puts a whole bunch of monsters into the Kokiri Forest. Then, he puts all the gorons into cells. Next, he freezes the zoras and lowers the level of Lake Hylia. Then, he burns Kakariko Village. Then, once you awaken the sages and Zelda reveals herself as Sheik, he kidnaps her. Finally, you have a battle with him at the top of his black tower. Once you deal the final blow he uses the last of his power to destroy the tower. Finally, all his anger and rage cause the triforce of power to turn him into a giant creature. Pretty freaking awesome if you ask me!