This article contributes to the growing body of research that focuses on the microfoundations of organizational ambidexterity, that is, understanding what enables individuals to address the exploitation-exploration dilemma. One central challenge generated by ambidexterity is the multiplicity and divergence of organizational roles, to which individuals need to cater when exploiting and exploring. Specifically, we point to the relevance of how individuals identify with and enact this multiplicity of role demands. Following identity theory, we apply the logic of role integration and role segmentation, a foundational classification of how individuals cognitively manage role multiplicity. Further, as different role domains often require the interaction with other organizational functions, we test for the moderating effect of cross-functional coordination on the relationship between role segmentation and individual ambidexterity. Based on data from 120 global account managers employed by multinationals with an average size of 73,348 employees, our results indicate that role segmentation negatively influences an individual’s ability to behave ambidextrously. Interestingly, though, when operating in cross-functional teams, the impact of role segmentation becomes positive. We conclude by highlighting the scope and significance of these findings for theory, managerial practice, and future research.