Herein, we have demonstrated a novel polymer network strategy-polyCATs-that allows us to combine the control of homogeneous catalysis with the benefits of heterogeneous catalysts through decoupling catalyst incorporation and environment (within the pores of MOC junctions) from the physical properties of the support (polymer strands). Two different CLs (TEMPO-CL and Au-CL) and three different PLs (PEG-PL, PS-PL, PBA-PL) were used to demonstrate the versatility and modularity of this approach using mechanistically distinct reactions. PolyCATs provided high reaction conversions in each test case, and they could be easily recycled and reused over subsequent reaction cycles, requiring only simple washing between reactions. Additionally, due to the distinct nature of polyCAT junctions versus strands, polyCATs allow recyclable catalysis in solvents where the traditional homogeneous catalyst is insoluble (e.g., H2O). In the future, the polyCAT strategy will leverage the diversity of MOCs of varied shape and composition available today, along with numerous polymer compositions, to facilitate the creation of catalytic materials for a range of synthetic endeavors, potentially simplifying organic synthesis, enabling novel cascade processes and greener manufacturing strategies, and ultimately achieving multifunctional materials that combine the robust mechanical properties of polymer networks with catalytic functions.