Which of the following two versions is correct? Or are both of them incorrect?
The one who ate all nuts was Squirrel.
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Both, kind of. It's an adverbial noun (noun that can behave like an adverb), so you can treat it like you would any other number + counter.
So your first sentence is almost correct (skip the に):
Alternatively, you can use の instead to use it attributively (but not な):