Traditionally, personality has been conceptualized in terms of dimensions of human experience – habitual ways of thinking, feeling, and behaving. By contrast, psychopathology has traditionally been conceptualized in terms of categories of disorder – disordered thinking, feeling, and behaving. The empirical literature, however, routinely shows that psychopathology does not coalesce into readily distinguishable categories. Indeed, psychopathology tends to delineate dimensions that are relatively similar to dimensions of personality. In this special issue of Personality Neuroscience, authors took up the challenge of reconceptualizing personality and psychopathology in terms of connected and interrelated dimensions, and they considered the utility of pursuing neuroscientific inquiry from this more integrative perspective. In this editorial article, we provide the relevant background to the interface between personality, psychopathology, and neuroscience; summarize contributions to the special issue; and point toward directions for continued research and refinement. All told, it is evident that quantitatively derived, integrative models of personality–psychopathology represent a particularly promising conduit for advancing our understanding of the neurobiological foundation of human experience, both functional and dysfunctional.