AbstractIn this work, state‐of‐the‐art Pd‐chelated poly(triazine imide) (Pd‐PTI) nanocatalysts were synthesized with PTI, as cheap solid support, and different Pd contents by an easy co‐precipitation method for conducting the model reduction reaction of p‐nitrophenol to p‐aminophenol. The electron microscopy observations (i.e., scanning electron microscopy and transmission electron microscopy), quantitative dispersive X‐ray spectroscopy and elemental mapping images demonstrated that Pd nanoparticles (NPs) were homogeneously loaded on the surface of highly crystalline two‐dimensional (2‐D) PTI nanosheets. Among the all prepared Pd‐PTI nanocatalysts, the PTI‐1500‐Pd indicated the highest pseudo‐first‐order rate constant of 12.7 × 10−3 s−1, which was significantly higher than that of the recently reported Pd‐based nanocatalysts. This catalyst showed ultrahigh, superior catalytic efficiency (≥99%) and stability properties for the hydrogenation of p‐nitrophenol within 40 s under mild conditions and possessed excellent recovery (≥90%) of expensive Pd NPs after five consecutive cycles. The high‐catalytic performance of the PTI‐1500‐Pd nanocatalyst is related to specific properties of the highly crystalline structure, high‐surface area and very available surface amine groups of 2‐D PTI nanosheets, which functioned as an active site for immobilizing ultrafine Pd0 NPs.