The lexically based five-factor model (FFM) of personality has been a highly influential research framework for characterizing clinical-psychological conditions, including psychopathy, in lexical-trait terms. An alternative trait-descriptive framework, the triarchic model was formulated to characterize psychopathy in neurobehavioral-trait terms, in order to facilitate linkages with variables in the domain of neurobiology. The current study used data from a mixed-gender sample (N = 769; M age = 19.3) to establish an interface between the FFM and triarchic frameworks by identifying subsets of items from a widely used five-factor personality inventory, the NEO Personality Inventory–Revised (NEO-PI-R), that effectively index the dimensional constructs of the triarchic model (boldness, meanness, and disinhibition). A consensus rating and psychometric refinement approach was used to select NEO-PI-R items for assessing each triarchic dimension, and the resulting NEO-Tri item-sets (“scales”) were evaluated in relation to criteria including other scale measures of the triarchic constructs, reported antisocial behavior and drug/alcohol use, and an FFM-generated omnibus psychopathy measure, the Psychopathy Resemblance Index. The NEO-Tri scales were also evaluated for effectiveness as indicators of latent triarchic dimensions within a confirmatory factor analysis anchored by previously validated triarchic scale measures. Results of this work have implications for clarifying how the triarchic model dimensions relate to normal-range personality traits and FFM-based conceptions of psychopathy, and provide a foundation for further examining neurobiological correlates of the triarchic model dimensions using existing multidomain data-sets that include the NEO-PI-R.