Psychopathology may be understood better as a spectrum, as opposed to a dichotomy, and the traits that underlie this spectrum can shed light on the underlying mechanisms of the pathology. The personality trait Neuroticism, which relates to the experience and expression of negative emotion, is strongly associated with psychopathology; the aspects of Neuroticism-N-Withdrawal and N-Volatility-share variance but are also uniquely associated with different types of psychopathology. Intelligence and creativity are two other traits that are associated with psychopathology; intelligence is negatively correlated, while creativity is sometimes positively correlated. Some of this correlation can be explained through their relationship to Neuroticism and its aspects. The current study examined the relationship between intelligence, creativity, and the aspects of Neuroticism, as well as explored potential neural mechanisms of Neuroticism. N-Volatility was negatively correlated with intelligence, while N-Withdrawal showed a curvilinear relationship, where subjects in the middle of the N-Withdrawal spectrum performed best on cognitive tasks. However, N-Volatility positively predicted creativity-particularly artistic creativity-in some samples, while N-Withdrawal showed no or a slight negative correlation. Finally, N-Withdrawal was negatively associated with functional connectivity in areas of the brain related to emotional regulation and decision making. These findings suggest that personality mediates the relationship between psychopathology, creativity, and intelligence, and imply a neural substrate of Neuroticism.