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Measuring treatment efficacy in individuals with Autism Spectrum Disorder (ASD) relies primarily on behaviors, with limited evidence as to the neural mechanisms underlying these behavioral gains. This pilot study addresses this void by investigating neural and behavioral changes in a Phase I trial in young adults with high‐functioning ASD who received an evidence‐based behavioral intervention, Virtual Reality‐Social Cognition Training over 5 weeks for a total of 10 hr. The participants were tested pre‐ and post‐training with a validated biological/social versus scrambled/nonsocial motion neuroimaging task, previously shown to activate regions within the social brain networks. Three significant brain‐behavior changes were identified. First, the right posterior superior temporal sulcus, a hub for socio‐cognitive processing, showed increased brain activation to social versus nonsocial stimuli in individuals with greater gains on a theory‐of‐mind measure. Second, the left inferior frontal gyrus, a region for socio‐emotional processing, tracked individual gains in emotion recognition with decreased activation to social versus nonsocial stimuli. Finally, the left superior parietal lobule, a region for visual attention, showed significantly decreased activation to nonsocial versus social stimuli across all participants, where heightened attention to nonsocial contingencies has been considered a disabling aspect of ASD. This study provides, albeit preliminary, some of the first evidence of the harnessable neuroplasticity in adults with ASD through an age‐appropriate intervention in brain regions tightly linked to social abilities. This pilot trial motivates future efforts to develop and test social interventions to improve behaviors and supporting brain networks in adults with ASD. Autism Res 2018, 11: 713–725. © 2018 The Authors Autism Research published by International Society for Autism Research and Wiley Periodicals, Inc. Lay Summary: This study addresses how the behavioral changes after treatment for ASD reflect underlying brain changes. Before and after receiving VR‐SCT, young adults with high‐functioning ASD passively viewed biological motion stimuli in a MRI scanner, tapping changes in the social brain network. The results reveal neuroplasticity in this age population, extending the window of opportunity for interventions to impact social competency in adults with ASD. [ABSTRACT FROM AUTHOR]