This study compared 143 law enforcement officers with a history of serious misconduct and 429 matched comparators who had completed the Candidate and Officer Personnel Survey–Revised (COPS–R), an inventory developed specifically for psychological evaluation of public safety candidates. Most had also completed the Personality Assessment Inventory (PAI), which allowed for scoring of scales and indices from the PAI Police and Public Safety Report (PAI-PPSR), as well as the recently developed PAI-Plus. Correlations and t tests indicated significant small group differences on seven COPS–R scales and one PAI-Plus index. Analyses were repeated for officers with substance use-related problems compared with nonproblem officers. These identified four COPS–R and two PAI-PPSR scales that were significant predictors. Relative risk ratio analyses indicated the clinical utility of these scales at certain cutoff scores in predicting serious misconduct in law enforcement officers and candidates. (PsycInfo Database Record (c) 2022 APA, all rights reserved)