The development of heterogeneous nanocatalysts with high performance is essential for improving hydrogen production through formic acid dehydrogenation, but challenging. Herein, highly dispersed Pd nanoparticles (NPs) were successfully immobilized on porous nitrogen-doped carbon cages (PNCCs) derived from zeolitic imidazole frameworks. By virtue of the synergistic effect, the optimized Pd/PNCC nanocatalytic systems exhibit an excellent catalytic kinetics toward catalyzing FA dehydrogenation with a turnover frequency (TOF) value as high as 3174 h⁻¹ at 323 K, which is 59 times relative to that of Pd nanoparticles. The exceptional activity may be ascribed to the PNCC solid support may induce a strong electronic metal–support interaction to optimize the electron configuration of Pd active sites and accelerate the kinetics of O-H bond cleavage, resulting in an enhanced catalytic performance toward FA dehydrogenation. This work will supply a novel strategy for the development of supported nanocatalysts with high performance for tremendous catalytic applications in the future.