Meeting the Prerequisites
Defeat the Elite Four. The Legendary Beasts only appear in the later stages of the game. You will need to defeat the Elite Four before you can find them.
Capture at least 60 species. You will need to do this in order to get the National Pokedex. Keep in mind that they need to be 60 unique Pokemon.
Get the National Pokedex. Catching 60 unique Pokémon will trigger an event at Professor Oak’s house. Go speak to him, and he will give you the National Pokedex.
Finding the Legendary Beasts
Use Max Repels. The Legendary Beasts roam the Kanto region at random, so finding them requires a lot of wandering through the grass with your fingers crossed. Using Max Repel will help you avoid endless encounters with low-level Pokémon while you do so. Make sure the first Pokémon in your party is level 49 or below, or this won’t work.
Hop on your bike. This is pretty straightforward. Riding your bike rather than walking will help you find Pokémon more quickly, as you will encounter more Pokémon in a smaller amount of time. With any luck, one of them will be a Legendary Beast.
Track it on your Pokedex. If you finally track down a Legendary Beast and it gets away from you, don’t despair. It will now show up in the map in your Pokedex, which will make the process of finding it much quicker. The Legendary Beast’s location will change every time you fly, battle, go into a building, or change routes. This may seem like a hindrance, but you can use it to your advantage. Hop on your bike, pop a Max Repel, and start trekking through the grass. If you haven't had a hit after about 30 seconds, head into the house. When you come back out, the Legendary Beast’s area of roaming will have changed. Rinse and repeat until it appears before you.
Catching the Legendary Beasts
Know what you’re up against. Only one of the three Legendary Beasts will appear in each game, and which one it is will depend on the player's choice of a starter Pokemon. The Legendary Beast in your game will always be the type that is super effective against your starter, so if you chose Squirtle it will be Raikou, if you chose Bulbasaur it will be Entei, and if you chose Charmander it will be Suicune. Plan your party accordingly. Raikou is an electric Pokemon, so ground types will be strongest against it, while water and flying types will be weak. Entei is a fire Pokemon, so water, ground, and rock types will be strongest against it, while grass, ice, bug, and steel types will be weak. Suicune is a water Pokemon, so grass and electric types will be strong against it, while fire, ground, and rock will be weak.
Stock up on Ultra Balls. You will need these to successfully catch a Legendary Beast. It will be difficult to catch, so pick up around 15 to be safe.
Keep it from fleeing. The Legendary Beasts are skittish, and they will always attempt to flee rather than engaging in battle. The best strategy is to use a move like Curse, Mean Look, or Block. Sleep or Freeze will also work, but since status effect moves like those are temporary, they’re not the best strategy. Alternatively, you can simply throw an Ultra Ball at it. Your chances are very small here, though, as the Legendary Beast will just probably escape the Pokeball and flee.
Battle it. Once you’ve found a way to keep the Legendary Beast from fleeing, the process of capturing it is the same as with any other Pokemon. Reduce its HP as much as you can without knocking it out, throw an Ultra Ball at it, and cross your fingers. Save frequently as you go, because if you accidentally knock out the Legendary Beast, you will not have another opportunity to catch it.
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