Mordenite nanosheet (NS-MOR) with flower-like morphology and high specific surface area was synthesized by using lab-made high-molecular a copolymer containing quaternary ammonium groups as a template, and employed for the prepared loading Pd (Pd/NS-MOR) catalyst by ion-exchange method. The zeolite and its supported-Pd catalyst were characterized by X-ray powder diffraction, N2-physical adsorption, SEM, TEM and X ray photoelectron spectroscopy. The results showed that Pd0 and Pd2+ species with small size were highly dispersed on the surface of nano-zeolite in the Pd/NS-MOR catalyst, while there were only Pd2+ species in the γ-Al2O3 supported Pd (Pd/γ-Al2O3) catalyst. Therefore, 2-phenylpyridine and benzaldehyde were used as raw materials, realizing the simultaneous activation of C2—H and C6—H bonds of 2-phenylpyridine. Pd/NS-MOR catalyst showed much higher catalytic activity and selectivity of diacylated products (92%) than Pd/γ-Al2O3 in C—H bond activation of 2-phenylpyridine with benzaldehyde. As a contrast, the diacylated products cannot be obtained in the homogeneous Pd(NO3)2, Pd(OAc)2, Pd(PhCN)2Cl2 catalytic system in C—H bond activation of 2-phenylpyridine. In addition, Pd/NS-MOR catalyst not only had good substrate compatibility, but also exhibited good 2-phenylpyridine conversion (95%) and diacylated products selectivity (85%) after the sixth cycle.