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To further understand the role of drinking to cope (DTC) motivation in the development of drinking-related problems during young adulthood, we tested whether the association between episode-specific levels of nighttime DTC motivation and next-day negative affect and self-control depletion symptoms (SCDS) changed from college years to postcollege years (5 years later). We also examined whether these changes were moderated by recent life stress, adult social role attainment and gender, and whether mean levels of these variables were associated with changes in drinking-related problems from college to postcollege years. Participants (N = 927; 54% women) completed a 30-day daily diary during college and again 5 years later in which they reported their previous night’s drinking level and motivation and their current negative affect and SCDS. We assessed drinking-related problems at both waves and recent life stress and adult social roles at Wave 2. DTC motivation was positively associated with next-day levels of negative affect and SCDS. The effect of DTC motivation on anxiety and SCDS became stronger over time. The effect of DTC motivation on depressive affect and anger (a) decreased across time among individuals who attained more adult roles and (b) was weaker among individuals who reported lower levels of postcollege life stress. Mean levels of postcollege DTC motivation was indirectly related to changes in drinking-related problems from college to postcollege through mean levels of negative affect and SCDS. Our findings indicate that DTC might exert its unique long-term effects on alcohol use disorders through disruption of daily emotion-regulation processes.