Shifts in governance can be conceived of as a response to policy capacities being shared—in a material sense—between centralized and decentralized levels of government. A comparative case study is conducted of three conceptually different shifts in governance. Unclear responsibility relations lead to “paradoxes of decentralization,” in which the applied mode of governance blocks the intended improvements. Three case studies are presented to illustrate these mechanisms. There is no “best” way of decentralizing responsibilities; requirements of governance modes are ambiguous. The sharing of policy capacities between central and decentralized levels of governance requires internally inconsistent governance arrangements.