Hybridized materials frequently exhibit boosting performances greater than those of the individual components in functional applications because of intriguing synergistic effects. Nonetheless, the preparation of hybrid materials is often tedious, involving stepwise procedures with different synthesis approaches. To date, controlled synthesis of hybrid materials via a one-pot CVD process has rarely been explored. In this work, herein, we report successful synthesis of the MoS₂/VS₂ hybrid by in situ growing the MoS₂ microflowers on the VS₂ microflakes via a one-step CVD process for electrolytic hydrogen evolution reaction (HER) in an acid electrolyte. The MoS₂/VS₂ hybrid exhibits enhanced HER performances as opposed to the standalone pristine MoS₂ and VS₂. Such improvement may be due to the formation of lightly vanadium-doped MoS₂. First-principle calculations further show that vanadium dopants can effectively enhance the in-plane electrical conductivity and intrinsic activity of MoS₂ simultaneously. The proposed CVD strategy in this work is scalable, timesaving, and versatile and can be used to grow a great variety of hybrid materials for different fields, enabling the cost-effective utilizations of recently reported novel materials.