Decomposition of polymers by heterogeneous catalysts presents a promising approach for reuse of waste plastics. We demonstrated non‐hydrogenative decomposition of model polyolefins over proton‐form and metal (Cu, Ni) ion‐exchanged beta (BEA) zeolites at moderate temperatures (around 300 °C). Near complete polyolefin decomposition was observed in batch reactions monitored by thermogravimetric analysis, while decomposition at partial conversion was studied in flow reactions. Ni‐exchanged zeolites produced H2 at substantially higher rates (>10x) than other catalysts while also uniquely resisting deactivation over time. Application of the delplot formalism offered insights into the reaction network for polyolefin decomposition over Ni/BEA most notably that H2 is solely a primary product. We deduce that H2 production is catalyzed by activation of C−H bonds at ionic Ni sites, and H2 prevents buildup of polyaromatic coke species in Ni‐exchanged zeolites that deactivate Cu‐exchanged and protonic zeolites.