Catalytic hydrocracking of polyethylene to branched liquid fuels has drawn particular attention. Here, bifunctional Pt/Nb2O5 catalysts with different Pt loadings were prepared for polyethylene hydrocracking. It was found that the low‐loading Pt/Nb2O5 catalysts exhibited significantly higher catalytic activity than those of high‐loading Pt/Nb2O5 catalysts, with the 0.2Pt/Nb2O5 catalyst having the best catalytic performance (79.2% yield of liquid fuels (C5‐C19) with branched alkanes accounting for 85.2%). Detailed characterizations revealed that the activation of H2 played a crucial role in the efficient hydrocracking of polyethylene. The 0.2Pt/Nb2O5 catalyst, with highly dispersed Pt nanoclusters on the surface, facilitated the highly active Hδ‐ species formation, thereby enhancing hydrocracking activity. This work highlights the importance of H2 activation in the hydrocracking of polyethylene and provides insights for the design of efficient catalysts.