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The best way to capture a Legendary Pokemon is the same way to capture any other Pokemon. First get a pokemon that has an advantage over it, such as using a Hariyama against Regice (Fighting moves are super effective against Ice types). Lower the Legendary's HP as far as you can down to the red with super effective moves. Then, use a move that isn't very effective (such as Ice Beam (Ice type attacks are the only attacks that aren't very effective against Ice types)). When your opponent's HP is as low as you want it, put it to sleep, paralyze it, or freeze it (Regice can't be frozen). Then start throwing whatever balls you have.

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Q: How do you cach legendary pokemon?
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