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I've seen it being used as a noun for 'crystals' in a game and it's also been
used as a verb in the form of 'Kesshou!(crystallize!)' for a superhero
transformation call in Spielban.

Is simply saying Kesshou normal for using it as a verb or do you normally
attach -suru to make Kesshou a verb?
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question
verbs parts-of-speech
Is 結晶 a verb and a noun?
Are you thinking if one might say けっしょいます, けっしょって or something like that? Then
definitely no, 結晶 itself is a simple noun that never conjugates. (A crystal
maniac might try coining such a verb [using this
pattern](https://japanese.stackexchange.com/q/24351/5010) as a joke, but I
have never heard such a verb.) 結晶する is still ungrammatical. If you want to say
"to crystallize", it's 結晶 **化** する (works transitively and intransitively),
where 化 (か) is a suffix like _-ization_.

"結晶化!" is too long as a "transformation call", so 結晶 is a reasonable choice
for that. Just because it's used similarly to "変身!" does not mean it's a verb.
Shouting a pure noun is not strange even in English (e.g., "Attention!",
"Silence!")
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answer