By adjusting various Ru/M (M=Co, Ni) molar ratios, a series of highly dispersed bimetallic RuM alloy nanoparticles (NPs) anchored on MIL-110(Al) have been successfully prepared via a conventional impregnation-reduction method. And they are first used as heterogeneous catalysts for the dehydrogenation reaction of AB at room temperature. The results reveal that the as-prepared Ru 1 Co 1 @MIL-110 and Ru 1 Ni 1 @MIL-110 exhibit the highest catalytic activities in different RuCo and RuNi molar ratios, respectively. It is worthy of note that the turnover frequency (TOF) values of Ru 1 Co 1 @MIL-110 and Ru 1 Ni 1 @MIL-110 catalysts reached 488.1 and 417.1 mol H 2 min −1 (mol Ru) −1 and the activation energies (E a) are 31.7 and 36.0 kJ/mol, respectively. The superior catalytic performance is attributed to the bimetallic synergistic action between Ru and M, uniform distribution of metal NPs as well as bi-functional effect between RuM alloy NPs and MIL-110. Moreover, these catalysts exhibit favorable stability after 5 consecutive cycles for the hydrolysis of AB.