Molybdenum disulfide (MoS 2 ) is a promising material for energy and environmental applications. In this paper, we report the direct hydrothermal growth of MoS 2 on a Mo support and its application in the rarely explored electrochemical CO 2 reduction (EC CO 2 R) process. To investigate the effects of metal overlayers and the MoS 2 support, Au, Ag, and Cu were sputter-deposited on a MoS 2 electrode. Large amounts of CH 4 , C 2−3 hydrocarbons, and formate were produced via EC CO 2 R on bare MoS 2 . The introduction of a Au overlayer on MoS 2 enhanced the production of CO, methanol, and formate. Furthermore, the alkanes (C 𝑛 H 2𝑛+2 , 𝑛 = 2, 3) to alkenes (C 𝑛 H 2𝑛 , 𝑛 = 2, 3) ratio was dependent on the applied potential and overlayer metals. Notably, photoirradiation remarkably increased the CO and C 2 H 4 concentrations by 28-fold and 10-fold, respectively. These findings provide valuable insights for the development of MoS 2 -based materials for CO 2 recycling.