PokéBase - Pokémon Q&A
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I thought I read somewhere that it can help get Pokémon with similar natures when breeding, but I can't remember...

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If the first Pokémon in your party has Synchronize, you have a 50% chance of encountering a wild Pokémon with the same nature as your Sumchronizer. For example, if I have an Adamant Synchronize Abra at the front of my party, all wild Pokémon have a 50% chance of having an Adamant Nature.

This does not apply to roaming Pokémon, Pokémon revived from Fossils, or Pokémon in the Entree Forest.

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