Self-control enables people to regulate their emotions, desires, cognitions, and behaviors. We distinguish between two types of self-control (i.e., inhibitory/stop-control and initiatory/start-control), revised De Boer et al.'s stop/start-control scales (Study 1), and examined their value in predicting work-related behavior and emotion regulation among employees in a two-wave design (Study 2). The findings show that stop- and start-control have differential predictive validity: Stop-control relates negatively to counterproductive work behavior and positively to expressive suppression, whereas start-control relates positively to increasing challenging job demands (job crafting), cognitive reappraisal, and positive framing. Moreover, usefulness analyses supported the incremental validity of the narrow stop/start-control facets beyond general trait self-control. These findings illustrate the value of stop/start-control at work, further substantiate stop/start-control theory, and suggest organizations should take stop/start-control into account (e.g., in personnel selection, job design).