Rational design of highly efficient non-noble-metal catalysts for the selective hydrogenolysis of biomass platform compounds to produce fuels and fine chemicals is a key pursuit for the sustainable chemical industry. In this work, we report for the first time the synthesis of a Ni-supported germanosilicate zeolite (Ni-SCM-14) catalyst by a simple grinding method, showing both satisfactory yield (90.3%) and good stability in eight cycles for the hydrogenolysis of 5-hydroxymethylfurfural (HMF) to 2,5-dimethylfuran (DMF). Characterization revealed that Ni nanoparticles were highly dispersed on the SCM-14 zeolite with strong interactions. The synergistic effect of highly dispersed Ni hydrogenation sites and the weak acidity activation of the C−O bond provided by SCM-14 is considered to be the key to the efficient hydrogenolysis of HMF. This discovery opens up a new avenue for germanosilicate zeolite to activate the C−O bond.