Objective: Recent research regarding the Behavioral Rating Inventory of Executive Function, Adult Version (BRIEF-A), suggests a three-factor structure may be more appropriate than the two-factor structure proposed by BRIEF-A developers. The three-factor model proposed by Roth et al. (2013) includes two indices related to separate aspects of behavior: Emotion Regulation (ERI; Shift and Emotional Control subscales) and Behavioral Regulation (Revised, BRI-r; Inhibit and Self-Monitor subscales). The current study evaluated the validity of ERI and BRI-r based on relevant MMPI-2-RF Higher-Order scales. Method: Valid MMPI-2-RF and BRIEF-A profiles (n = 78) were collected from veterans evaluated at a VA neuropsychology clinic. Correlational analyses were performed with MMPI-2-RF Emotional/Internalizing Dysfunction (EID) and Behavioral/Externalizing Dysfunction (BXD) scales and the four subscales contributing to BRIEF-A ERI and BRI-r. Hierarchical regression evaluated unique contributions of EID and BXD to BRIEF-A subscales. Results: EID and BXD showed mild to moderate correlations with all ERI and BRI-r subscales. For the two ERI subscales, after EID was entered into the model (ps < .01), there was no significant contribution of BXD (p = .96, .19). For the two BRI-r subscales, after BXD was entered into the model (ps < .02), EID accounted for a significant degree of variance (ps < .01). Conclusion: All subscales contributing to BRI-r and ERI were associated with emotional/internalizing symptoms of the MMPI-2-RF, suggesting that BRI-r subscales are not specific to externalizing behaviors. In contrast, subscales contributing to ERI were not associated with behavioral/externalizing symptoms, suggesting the convergent and discriminant validity of ERI. Overall, results provide mixed support for the three-factor model proposed by Roth et al. (2013).