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Complete 400 Brawl Matches. Defeat Toon Link.

Article:
If you don't feel like playing through the single-player modes, you can unlock Toon Link by playing 400 multiplayer Brawl matches. You can play Brawl Matches against computer opponents or against other people, either locally or online. After the 400th match Toon Link will then challenge the winner to a Brawl. Once you defeat Toon Link one-on-one, you will be able to select him from the Character Select menu in any mode.