PokéBase - Pokémon Q&A
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You have to give them (or take away) either the Rusted Sword (for Zacian) or the Rusted Shield (for Zamazenta) to change forms. These items are obtained through the main story. Giving them their respective item will change them into their Crowned Formes, while taking them away will revert them to their Hero of Many Battles Formes.

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By holding Rusted Sword:

Changes a Zacian holding this item into its Crowned Sword form. In-battle, it also changes Zacian's Iron Head into Behemoth Blade.

Source

By holding Rusted Shield:

Changes a Zamazenta holding this item into its Crowned Shield form. In-battle, it also changes Zamazenta's Iron Head into Behemoth Bash.

Source

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