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In Ectreatek (Or that sort of city... sorry i forgot how to spell it) city you go to burn Tower. Then you unleash Suicune, Raikou and Entei. Raikou and Entei appear on your pokegear map so you have to follow them or raikou... If you have a masterball lucky you but if you don't, you can use an ultra ball. Obviously, it will take a lot of ultra balls to catch it but it will eventually give in. I've heard that if it's night time, you can use dusk balls. But this is only if it's night...

PS: this is Soul Silver.

AnswerWell, you have to find it first. You can get Raikou only in the FireRed and LeafGreen versions if your starter Pokemon was squirtle. After beating the Elite Four, it will be wandering around the grass in the Kanto Region (Once you've seen it, you can track it down with your Poke'dex). When you find it, throw your Master Ball. If you already used it, then you can put a Wobbuffet or Dugtrio or Trapinch first in your party, or use the move Mean Look or Block, so that it can't run away. Then throw Ultra Balls (If you weaken it and it runs away, then the next time you see it it will still have the same amount of HP as the last time you saw it). AnswerWell, you have to find it first. You can get Raikou only in the FireRed and LeafGreen versions if your starter Pokemon was squirtle. After beating the Elite Four, it will be wandering around the grass in the Kanto Region (Once you've seen it, you can track it down with your Poke'dex). When you find it, throw your Master Ball. If you already used it, then you can put a Wobbuffet or Dugtrio or Trapinch first in your party, or use the move Mean Look or Block, so that it can't run away. Then throw Ultra Balls (If you weaken it and it runs away, then the next time you see it it will still have the same amount of HP as the last time you saw it).
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