High-performance nano-MoS2-based catalysts for higher alcohol synthesis (HAS) through CO hydrogenation were synthesized using non-thermal plasma under ambient conditions. The as-synthesized catalysts were carefully characterized using XRD, BET, H-2-TPD/TPR, CO-TPD, in-situ CO adsorption DRIFTS, TEM, XPS, ICP, elemental analysis, and CO-TPSR techniques. The study results suggest that the non-thermal plasma approach not only achieves a large number of the small nano-MoS2 particles, but also decreases the synthesis time, compared to the conventional thermal methods. This flexible and facile approach can give the thinner and shorter MoS2 slabs, expose more coordinatively unsaturated sites, and increase the number of active centers for alcohols formation. Therefore, the non-thermal plasma-synthesized MoS2 -based catalysts exhibited the excellent catalytic performances for HAS.