A simple one-pot synthesis of Ni nanoparticle/ordered mesoporous carbon composite electrode materials is demonstrated for electrosynthesis for the first time. The obtained nanocomposites have uniform mesopore sizes (3.0-3.7 nm), large specific surface areas (506-633 m2 g-1), high pore volumes (0.28-0.38 cm3 g-1), well-graphitized carbon frameworks, and uniformly dispersed Ni nanoparticles (7-15 nm) embedded in the carbon pore walls. The prepared materials show very high performance in the selective (∼84%) electrocatalytic reduction of aromatic ketones into alcohols (∼79%).