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The purpose of this work is to investigate the controllability of non-instantaneous impulsive (NII) Hilfer fractional (HF) neutral stochastic evolution equations with a non-dense domain. We construct a new set of adequate assumptions for the existence of mild solutions using fractional calculus, semigroup theory, stochastic analysis, and the fixed point theorem. Then, the discussion is driven by some suitable assumptions, including the Hille–Yosida condition without the compactness of the semigroup of the linear part. Finally, we provide examples to illustrate our main result.