As employees’ personal lives are increasingly splintered by work demands, the boundary between work and nonwork domains is becoming ever more blurred. Grounded within a self-regulatory approach and the executive control function of inhibitory control, we operationalize and examine nonwork role re-engagement (NWRR)—the extent to which individuals can redirect attentional resources back to nonwork tasks following work-related intrusions. In phases 1 and 2, we develop and refine a psychometrically sound unidimensional measure for NWRR aligned with the self-regulatory processes of self-control and interference control underlying inhibitory control. In phase 3, we confirm the factor structure with a new sample. In phase 4 we validate the measure using the samples from phases 2 and 3 to provide evidence of criterion-related, convergent, and discriminant validity. NWRR was related to important well-being and work-related outcomes above and beyond existing self-regulatory and boundary management constructs. We offer theoretical and practical implications and an agenda to guide future research, as attentional agility becomes increasingly relevant in a home life replete with interruptions from work.