A central question in neuroscience is what visual features drive brain responses across regions. Classic approaches rely on handcrafted stimuli to test specific hypotheses, limiting discovery to features defined before experiments. Here we introduce NeuroVolve, a data-driven generative framework for synthesizing images that achieve flexible, user-defined patterns of brain activation in individuals. NeuroVolve recovers established selectivity across visual cortical regions and, paired with subject-specific brain encoding models, generates personalized stimuli reflecting individual differences in neural preference. Beyond single-region selectivity, NeuroVolve uncovers multi-region response selectivity, characterizing how regions jointly represent visual content during naturalistic perception. We further demonstrate generalization beyond visual cortex: in a prospective fMRI experiment, NeuroVolve-generated stimuli targeting the amygdala, a classically non-sensory region, drove measured activation consistent with predictions in novel participants. Together, these results establish NeuroVolve as a less constrained, data-driven tool for probing individual-level neural selectivity across the brain.

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