Catching Entei
Go to Goldenrod City and buy 20 Ultra Balls and 20 Dusk Balls. It's recommended to capture the three Legendaries at night in the game because this means you can use both Ultra Balls and Dusk Balls. Dusk Balls have a bonus catch rate if the time is 18:00-03:59 (6:00 p.m. - 3:59 a.m.)
Head to where Entei is (walk or run but do not fly!). After the encounter in the Burned Tower, you'll see both Entei and Raikou roaming on your map, so you can easily find them. You'll most likely need to go to an area where the city limits meet a route (any city, including Ecruteak City, Violet City, and GoldenRod City) and continuously run in and out of the city and check your map. Eventually, you'll see Entei close to you on the map and you can run over to his location. Walk in the tall grass to encounter Entei. You can also use the Repel item to prevent other Pokémon from appearing as you search the grasses for Entei.
Battle Entei. Entei is level 40 and has the moves Roar, Fire Spin, Stomp, and Flamethrower, so make sure you have a Pokémon that can take his hits. Entei will run from battle as soon as possible.
Use Snorlax's Block attack to ensure that Entei cannot escape. Since Entei immediately tries to run away from the battle, you'll need to stop that from happening. You can also use Mean Look to prevent Entei from running.
Start to throw Dusk Balls and Ultra Balls at Entei once it's HP is in the red zone or a low orange. You may have to throw multiple balls between attacks. You can use Snorlax's Crunch to weaken Entei. Then hold Leftovers to regain XP as Entei attacks.
Throw balls until Entei is captured or runs away. When the Pokémon reaches a low health meter, it will use Roar and run away. If Entei runs away, that's ok, go heal your Pokémon at the nearest Poké Center and return to where you last encountered Entei. You'll have to search for him again, but his health will be the same as when he ran away last time.
Catching Raikou
Go to Goldenrod City and buy 20 Ultra Balls and 20 Dusk Balls. It's recommended to capture the three Legendaries at night in the game because this means you can use both Ultra Balls and Dusk Balls. Dusk Balls have a bonus catch rate if the time is 18:00-03:59 (6:00 p.m. - 3:59 a.m.) The process to catch Raikou is identical to catching Entei.
Head to where Raikou is (walk or run but do not fly!). After the encounter in the Burned Tower, you'll see both Entei and Raikou roaming on your map, so you can easily find them. You'll most likely need to go to an area where the city limits meet a route (any city, including Ecruteak City, Violet City, and GoldenRod City) and continuously run in and out of the city and check your map. Every time you run out of the city's limits, you'll see on your map that Raikou is in a different area. Repeat this process of running in and out of the city's limits until you see Raikou close to you on the map and you can run over to his location. Walk in the tall grass to encounter Raikou. You can also use the Repel item to prevent other Pokémon from appearing as you search the grasses for Raikou.
Battle Raikou. The Legendary Pokémon is level 40 and has the moves Roar, Quick Attack, Spark and Reflect, so make sure you have a lead Pokémon that can take his hits. Raikou will run from battle as soon as possible.
Use Snorlax's Block attack to ensure that Raikou cannot escape. Since Raikou immediately tries to run away from the battle, you'll need to stop that from happening. You can also use Mean Look to prevent Raikou from running.
Start to throw Dusk Balls and Ultra Balls at Raikou once it's HP is in the red zone or a low orange. You may have to throw multiple balls between attacks. You can use Snorlax's Crunch to weaken Raikou. Then hold Leftovers to regain XP as Raikou attacks.
Throw balls until Raikou is captured or runs away. When the Pokémon reaches a low health meter, it will use Roar and run away. If Raikou runs away, that's ok, go heal your Pokémon at the nearest Poké Center and return to where you last encountered Raikou. You'll have to search for him again, but his health will be the same as when he ran away last time.
Catching Suicune
Go to the house north of Cianwood City. Suicune is to the right of the house at the north of this island but will vanish when you get close. Suicune isn't like Raikou or Entei since it can't be caught randomly. You have to go to certain locations to encounter Suicune before you can capture it. You also don't need to prevent Suicune from running from battle, so you won't need your Snorlax or Gengar.
Go to Route 42, outside Mt. Mortar. You should be able to surf west a bit and find a tree you can cut. It will lead you to a small grove with three trees with berries in the middle. Suicune will be there, but will again run away when you get close.
Go to Vermillion City. Suicune will be there on the port leading off of the S.S. Aqua, but will disappear when you get close.
Go to Route 14 of Kanto. It's towards Route 13.
Go to Cerulean City. You'll find Suicune next to Bill's house on Route 25 after you've defeated Misty and she returns to her gym.
Battle Suicune. The Legendary Pokémon is level 40 and has the moves Rain Dance, Gust, Aurora Beam and Mist, so make sure you have a lead Pokémon that can take his hits.
Throw Dusk Balls and/or Ultra Balls until Suicune is captured. Since Suicune is a Water-type Pokémon, you'll want to use a Grass, Water, or Dragon-type Pokémon. Use False Swipe to keep Suicune at 1 HP, so you don't accidentally defeat it. If you defeat Suicune, that's ok, go heal your Pokémon at the nearest Poké Center and return to the burned tower.
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