Green and highly selective synthesis of organonitrogen chemicals (ONCs) using the renewable energy source biomass over noble-metal free solid catalysts under common room temperature and pressure conditions is still a major challenge. Here, we report a sustainable electrochemical method for selective synthesis of several valuable ONCs with high yields using biomass-derived furanic aldehydes over greenly fabricated TiS2 nanosheets through a facile synthesis. Based on a range of characterization techniques including high-resolution transmission electron microscopy and X-ray absorption fine structure, a well-defined structure of the TiS2 nanosheets (3.86 nm with 1T phase) was constructed. These as-prepared catalysts were applied to the electrochemical reductive amination (ERA) of three biomass-derived aldehydes, i.e. furfural (FF), 5-methylfurfural (MF) and 5-hydroxymethylfurfural (HMF), and exhibited superior performance whereby over 95% conversion of each furanic aldehyde and nearly perfect selectivity of ONCs were achieved. TiS2 nanosheets, in particular, exhibited a marked ∼2-fold increase in conversion (∼49%) compared with the monometallic Ti electrode. Besides, the reaction kinetics and rational pathway were also studied. In addition, these exfoliated TiS2 nanosheets maintained high durability over 6 h, providing a promising and versatile route for the sustainable upgrading of biomass-derived sources.