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More and more self-interested businesses are organizing themselves in interdependent, non-hierarchically controlled networks to jointly create superior value by engaging in open innovation projects. In aligning the heterogeneous actors toward a focal value proposition, it is crucial for the orchestrators of such arrangements to manage their inter-organizational relationships by navigating the interplay of contractual and relational governance mechanisms. Despite the relevance of how contracts and relational governance co-evolve, knowledge on the interaction of contracts and relational governance in specific contexts is still missing. Through a multiple-case study of ten multinational ecosystem orchestrators, we explore how large multinational orchestrators govern the interplay inter-organizational relationship mechanisms in open innovation projects across ecosystems. Based on our findings, we propose a five-dimensional, sequential model of governing the interplay of inter-organizational relationship mechanisms in open innovation projects across ecosystems and discuss our contributions in the context of the current literature.