The development and refinement of psychopathy represent a critical issue in clinical and forensic practice. During the last decade, important advances in the operationalization of psychopathy were achieved, primarily through the development of the Psychopathy Checklist (PCL) and its subsequent versions (PCL-R and PCL:SV). PCL ratings are based primarily on item descriptions or subcriteria. The current study serves to break new ground as the first systematic investigation of PCL:SV subcriteria by addressing their psychometric properties and exploring their construct and criterion-related validation. Previously unanalyzed data from three samples were integrated: female offenders, male forensic patients, and male adolescent offenders. Results largely support the use of subcriteria as homogeneous components of criteria and provide strong initial evidence of their construct validity. Results are less conclusive regarding criterion-related validity. For female offenders, they suggested the potential value of specific PCL:SV subcriteria for predicting verbal aggression. Confirmatory factor analysis provided encouraging results on the applicability of the standard two-factor model of psychopathy. However, a first-order principal axis factoring suggested further refinements in our understanding of psychopathy.