This study by Ciesielski, Hou, and Samorì et al. successfully constructed a synergistic catalytic system between COF frameworks and metal oxides through a molecular-level supramolecular engineering strategy. This breakthrough not only provides a novel solution to address the kinetic bottleneck of acidic OER but also validates the unique advantages of COFs as a customizable platform for constructing complex proton transport networks and regulating reaction intermediate adsorption behaviors. With the optimization of synthesis processes and exploration of alternative metal centers, this system holds significant potential to substantially reduce PEMWE hydrogen production costs and accelerate the advent of the green hydrogen economy era.