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Here are the most recommended steps on catching Raikou are:

  1. Bring a Pokemon with you that have the move Yawn, Hypnosis, Sing, or Sleep Powder and Mean Look. I recommend Yawn after using Mean Look to prevent it escaping and it has 100% accuracy.
  2. Bring many Ultra Balls if you can or Great Balls at least. I recommend bringing a Timer Ball for long battles, but that's not required! It's just easier!
  3. Encounter Raikou again and make sure your Pokemon with Mean Look is up front with a really high level. This will ensure your Pokemon to move first. After Mean Look is used, switch out your Pokemon to the one with the sleep-inducing move.
  4. Let your Pokemon use any of the sleeping moves, then damage Raikou till it's down to at least in yellow. Red is recommended, but it can be risky trying to get it to that low.
  5. Throw many Ultra Balls, about 5 of them, then throw an Timer Ball. Repeat till you capture it.
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10y ago

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Hints of catching raiku?

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