The facile catalytic reversible (de)hydrogenation of liquid organic hydrogen carriers (LOHC) using a single catalyst holds great value for onboard hydrogen storage. Herein, we develop a bimetallic catalyst Pd1Ni based on nonnoble metal Ni with ultralow Pd of 0.05 wt%, which enables reversible (de)hydrogenation of NPC and supports multiple cycles of reversible hydrogen uptake and release. Notably, the bimetallic catalyst Pd1Ni exhibits more excellent catalytic performance on the dehydrogenation reaction of dodecahydro-N-propylcarbazole (12H-NPC) than the 1%Pd catalyst and similar catalytic performance on the hydrogenation reaction of NPC compared to the 1%Ru catalyst. The astonishing catalytic efficiency of Pd1Ni catalysts is due to the ideal electronic structure between ultralow Pd and Ni NPs allowing rapid interfacial electron transfer to intermediates, as revealed by structural analyses and density functional theory (DFT) computations.