In the psychological science field, there is substantial interest in quantifying individual differences in self-regulatory capacity because of its transdiagnostic relevance to various forms of psychopathology. Trait disinhibition and impulsiveness are popular conceptualizations of dispositions reflecting self-regulation of behavioral and emotional responding. In the literature, these constructs are often treated interchangeably because of their shared focus on general disconstraint and a lack of direct comparisons between measures of each. The current work used structural modeling to examine conceptual and empirical differences between 2 popular operationalizations of these traits in 2 samples (Ns = 400, 308), and employed regression and dominance analyses to compare their predictive relations with criterion measures of externalizing problems and negative affectivity (NA). Impulsigenic traits were related both to externalizing problems and NA, whereas trait disinhibition was selectively associated with externalizing. In a dominance analysis, trait disinhibition exhibited complete dominance over all impulsigenic traits in predicting externalizing problems. Conversely, multiple impulsigenic traits evidenced complete dominance over trait disinhibition in prediction of NA. The current work provides evidence that (a) disinhibition and impulsigenic traits are not interchangeable, (b) disinhibition specifically indexes propensity for externalizing problems, and (c) impulsigenic traits reflect a blend of externalizing and NA that appears relevant to diverse forms of psychopathology. (PsycInfo Database Record (c) 2021 APA, all rights reserved).