Go to Victory Road. You must first catch a Deino, which can be found on the 1st and 3rd floors of Victory Road by walking, and it has a 20% of showing up. The location of Deino is the same in both Black and White.
Carry a Pokémon with you that has status-affecting moves such as Thunder Wave or Hypnosis. It would also be wise to have a Pokémon who knows the move False Swipe. No matter how strong your Pokémon is, the move False Swipe will always leave the target with at least 1 hp.
Carry some Ultra Balls or Dusk Balls. Dusk Balls are very effective at night, or in dark places such as caves.
Carry some Potions as well. Wild Pokémon may surprise you by having high-damage dealing attacks.
Once you come across one, try using False Swipe to lower it's hp down and then putting it to sleep. Beware of moves that burn or poison, as they will drain the Deino's life, possibly before you can capture it.
Once you have your Deino, start leveling! Deino doesn't evolve into Zweilous until level 50.
Zweilous doesn't evolve until level 64, at which point, you will have your pseudo-legendary!
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