Individual differences in attentional control involve the ability to voluntarily direct, shift, and sustain attention. In studies of the role of attentional control in emotional adjustment, social relationships, and vulnerability to the effects of stress, self-report questionnaires are commonly used to measure this construct. Yet, convincing evidence of the association between self-report scales and actual cognitive performance has not been demonstrated. Across 2 independent samples, we examined associations between self-reported attentional control (Attentional Control Scale; ACS), self-reported emotional adjustment, Five-Factor Model personality traits (NEO Personality Inventory-Revised) and performance measures of attentional control. Study 1 examined behavioral performance on the Attention Network Test (ANT; Fan, McCandliss, Sommer, Raz, & Posner, 2002) and the Modified Switching Task (MST; Suchy & Kosson, 2006) in a large sample (n = 315) of healthy young adults. Study 2 (n = 78) examined behavioral performance on standardized neuropsychological tests of attention, including Conner's Continuous Performance Test-II and subtests from the Wechsler Adult Intelligence Scales, Third Edition (WAIS-III; Psychological Corporation, 1997) and Delis-Kaplan Executive Function System (D-KEFS; Delis, Kaplan, & Kramer, 2001). Results indicated that the ACS was largely unrelated to behavioral performance measures of attentional control but was significantly associated with emotional adjustment, neuroticism, and conscientiousness. These findings suggest that although self-reported attentional control may be a useful construct, researchers using the ACS should exercise caution in interpreting it as a proxy for actual cognitive ability or performance.