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I examine the path-dependent processes that lead to changes in the institutional architectures of international regime complexes over time and analyze the effects on dynamics of contestation and behavioral adjustment by component institutions and actors. Specifically, I investigate how a gradual erosion of hierarchy and functional differentiation within the regime complex for nuclear non-proliferation (NNP) contributed to institutional contestation through regime shifting and rival regime creation. Over time, these undermined legal frameworks and weakened behavioral adjustment by state parties. While the unravelling of legal frameworks was partly a result of exogenous factors—including the emergence of new technologies and new actors—this paper shows that institutional proliferation and contestation have also been shaped by the very structure of the regime complex and are, as such, endogenous to cooperative frameworks. The analysis traces how legal frameworks from the Treaty on Non-Proliferation of Nuclear Weapons (1970) through the Nuclear Ban Treaty (2017) channeled (exogenous) dissatisfaction into particular patterns of contestation and behavioral adjustment, which in turn shaped successive institutional arrangements. Contrary to expectations of others, the paper finds that the NNP complex became less hierarchical and differentiated over time, caught in a ‘negative feedback loop’ in which fragmentation encouraged forum shopping and regime creation, reducing compliance and triggering another round of fragmentation.