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N-ethylcarbazole (NEC) is one of the most promising liquid organic hydrogen carriers (LOHCs) due to its low dehydrogenation enthalpy. The development of an efficient catalyst for the dehydrogenation of dodecahydro-N-ethylcarbazole (H 12 -NEC) is the key to the large-scale application of LOHCs. In this paper, Ni/MCM-41 was prepared by chemical reduction method using MCM-41 as the carrier, and then MCM-41 loaded Ni n @Pd 1 core-shell nanocatalysts (Ni n @Pd 1 /M41) were prepared by ultrasound-assisted galvanic replacement method using Ni as the templating agent and reducing agent. It was shown that there was electron transfer between Ni and Pd, and SMSI effect of Ni n @Pd 1 with MCM-41 by the characterization results of Ni n @Pd 1 /M41, which promoted the catalytic performance. H 12 -NEC dehydrogenation efficiency over Ni 6 @Pd 1 /M41 reached 100% at 180 °C for 4 h and at 170 °C for 6 h, and 97.58% for 6 h at 160 ℃, and TOF was 5080.6 h−1, which was better than that reported in the literature. The excellent catalytic dehydrogenation performance of Ni 6 @Pd 1 /M41 can mainly be attributed to the synergistic effect of coordination and strain effects between the bimetals. [Display omitted] • Ni n @Pd 1 /M41 core-shell catalysts for H 12 -NEC dehydrogenation were prepared by ultrasound-assisted galvanic replacement. • Coordination and strain effect between Ni and Pd, SMSI effect of Ni n @Pd 1 with MCM-41 improved the catalytic performance. • H 12 -NEC dehydrogenation efficiency over Ni 6 @Pd 1 /M41 reached 100% at 180 ℃ for 4 h and at 170 ℃ for 6 h. • TOF of H 12 -NEC dehydrogenation over Ni 6 @Pd 1 /M41 was 5080.6 h−1. [ABSTRACT FROM AUTHOR]