<p>Extant research has examined the moderating effects of contingency factors—such as green knowledge processing capability, organizational maturity stage, and firm age—on the positive relationship between sustainability orientation and performance. Research suggests that organizations with a sustainability orientation require certain capabilities to support the implementation of sustainable practices. However, limited attention has been given to explaining the development of such capabilities from a microlevel perspective that considers employees’ cognition and behavior. Drawing on the theory of locus of control, we explore how employees with different levels of control (ILOC versus ELOC) respond cognitively and behaviorally to sustainability orientation. The findings of two studies, a scenario-based experiment (Study 1) and a three-wave, multisource survey (Study 2), reveal that organizational sustainability orientation shapes employees’ attitudes and motivations toward sustainable tasks, which in turn influence their sustainable behavior. Specifically, individuals with an ILOC, characterized by a heightened sense of personal control and a mature capacity for moral reasoning, are more inclined to imbue their work with moral considerations and thus engage in innovative sustainability practices. Conversely, individuals with an ELOC tend to prioritize immediate financial gains, instrumentalizing their sustainable tasks and resorting to expediency. This research contributes to the literature by uncovering the cross-level psychological mechanisms through which sustainability orientation influences employee behavior. It also extends the current understanding of the antecedents of work moralization and job instrumentality, offering practical insights for enhancing the effectiveness of sustainability orientation implementation in organizations.</p>