Although research on organizational ambidexterity has exploded in the past several years, the determinants of individual‐level ambidexterity have received little scholarly attention. This is surprising given that management scholars increasingly highlight the benefits of combining explorative and exploitative activities in individual employees’ work roles. Using data collected by a two‐wave survey of 638 employees nested in 173 groups across 34 organizations, our research demonstrates that both psychological factors and leadership predict employees’ ambidextrous behaviour. Our results demonstrate that general self‐efficacy positively predicts ambidextrous behaviour through learning orientation. In addition, we show that employees exhibit higher ambidexterity when their group managers demonstrate paradoxical leadership; that is, a leadership style that couples strong managerial support with high performance expectations. Paradoxical leadership also moderates the relationship between learning orientation and individual ambidexterity such that employees’ ambidextrous behaviour is highest when paradoxical leadership and employee learning orientation are simultaneously at high levels.