question: Need for closure (NFC) reflects stable individual differences in the desire for a quick, definite, and stable answer to a question. A large body of research has documented the association between NFC and various cognitive, emotional and social processes. Despite considerable interest in psychology, little effort has been made to uncover the neural substrates of individual variations in NFC. Herein, we took a data-driven approach to predict NFC trait combining machine learning framework and the whole-brain grey matter volume (GMV) features, which represent a reliable brain imaging measure and have been commonly employed to explore neural basis underlying individual differences of cognition and behaviors. Brain regions contributing to the prediction were then subjected to functional connectivity and decoding analyses for a quantitative inference on their psychophysiological functions. Our results indicated that multivariate patterns of GMV derived from multiple regions across distributed brain systems predicted NFC at individual level. The contributing regions are distributed across the emotional processing network (e.g., striatum), cognitive control network (e.g., lateral prefrontal cortex), social cognition network (e.g., temporoparietal junction) and perceptual processing network (e.g., occipital cortex). The current study provided the first evidence that dispositional NFC is embodied in multiple large-scale brain networks, helping to delineate a more complete picture about the neuropsychological processes that support individual differences in NFC. Beyond these findings, the current interdisciplinary approach to constructing and interpreting neuroimaging-based prediction model of personality traits would be informative to a wide range of future studies on personality. Supplementary Information The online version contains supplementary material available at 10.1007/s11682-021-00574-w.