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To optimize the disadvantage of low conductivity and few active sites of MoS 2 -based catalysts, in situ growth on carbonized wood (CW) through coupling of conductive materials and MoS 2 can be a proven strategy. Herein, a three-dimensional self-supporting electrode with a heterostructure of nanosheet MoS 2 -decorated MoO 2 grown on CW (MoS 2 -MoO 2 /CW) is prepared for the hydrogen evolution reaction (HER) via a simple two-step chemical vapor deposition strategy. The coupling of MoS 2 and MoO 2 with excellent electrical conductivity and the rational design of three-dimensional self-supporting electrodes are the key factors to improve the catalytic performance. The designed MoS 2 -MoO 2 /CW electrode has a potential of 148 mV at a current density of 10 mA cm −2 , a low Tafel slope of 86.7 mV dec −1 , and outstanding long-term stability in 0.5 M H 2 SO 4 . Consequently, wood-based porous carbon electrodes with a heterogeneous structure of nanosheet MoS 2 -decorated MoO 2 can provide meaningful references for MoS 2 -based electrocatalysts.