Catch a Sneasel/Scyther, evolve it into a Weavile/Scizor and teach it False Swipe. False Swipe does decent damage for a 40PP move, but always leaves the Pokémon with 1HP.
Catch a Gastly and teach it Hypnosis. Hypnosis sends the Pokémon to sleep, making it incapable of attack and easier to catch. (Although Pokémon roaming around the map may still flee.) If you are planning to catch a roaming Pokémon (Mesprit, Latias, etc.) teach Gastly Mean Look, which prevents wild Pokémon from escaping.
Level up your Pokémon as high as you can.
Buy as many Ultra Balls as you can. (Although some Pokémon may be better caught with others. Case in point, Groudon is the heaviest Pokémon ever so will be most vulnerable to Heavy balls.)
Go find that Legendary!
Engage the Pokémon in battle and use False Swipe to whittle down it's HP and use Hypnosis to send it to sleep.
Keep throwing Ultra Balls (or whatever you have) until the Pokémon is yours.
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