This study proposes top management team (TMT) shared leadership as an important enabler of organizational ambidexterity. Moreover, we examine both how and when TMT shared leadership enhances organizational ambidexterity by considering two TMT processes as mediators (i.e., cooperative conflict management style and decision-making comprehensiveness) and two elements of organizational structure (i.e., connectedness and centralization of decision making) as important contingencies. We test our moderated mediation framework using time-lagged data from a cross-industry sample of 202 firms. We discuss how our findings extend strategic entrepreneurship, ambidexterity, and leadership research and provide implications for practice. © 2013 Strategic Management Society.