Organizational Sustainability is an increasingly important movement in the business world because of its social impact and also for the obligations imposed by state agendas and programs by global entities, such as the United Nations. At the forefront of such a movement is the Human Resources function, given its boundary activities with several critical internal and external stakeholders. The term Green Human Resource Management (GHRM) has been used to describe people management with a focus on green issues. The main objective of this research was to explore the relationship between personal values associated with sustainable behaviors (altruistic, biospheric, egoistic, and hedonic values), organizational outcomes such as engagement and commitment, and GHRM. A questionnaire was prepared and used to collect 532 responses from employees from various organizations. Results show that of the four personal values only the biospheric one moderates the relationship between GHRM practices and affective commitment so that the relationship between HRM and affective commitment is stronger when biospheric values score higher. This is an important finding, as it shows that when people value the biosphere, the effect of GHRM practices on affective commitment and work engagement is stronger than when people value other matters.