While a considerable number of youth with autism spectrum disorder exhibit impaired self-regulation (dysregulation), little is known about the neural correlates of dysregulation in autism spectrum disorder. In a sample of intellectually able boys with autism spectrum disorder (further categorized as those with and without dysregulation) and typically developing boys (aged 7-17 years), we conducted a multivariate connectome-wide association study to examine the intrinsic functional connectivity with resting-state functional magnetic resonance imaging. Dysregulation was defined by the sum of Attention, Aggression, and Anxiety/Depression subscales on the Child Behavior Checklist. We identified that both categorical and dimensional neural correlates of dysregulation in youth with autism spectrum disorder involved atypical connectivity among the components of multiple brain networks, especially between those subserving sensorimotor processing and salience encoding, beyond higher-level cognitive control circuitries. Interaction within the attention network might serve as autism spectrum disorder--specific neural correlates underpinning dysregulation. Our results highlight that the inter-individual variability in dysregulation might contribute to the inconsistency in the neuroimaging literature of autism spectrum disorder. Collectively, the present findings provide evidence to suggest that dysregulation might be considered as both categorical and dimensional moderators to parse heterogeneity of autism spectrum disorder.