As a new paradigm of material science, two-dimensional (2D) heterostructured composites have attracted extensive interests because of combining the collective advantages and collaborative characteristics of individual building blocks. Molybdenum disulfide (MoS₂) has demonstrated great promise as a low-cost substitute to platinum-based catalysts for electrochemical hydrogen production. However, the broad adoption of MoS₂ is hindered by its limited number of active sites and low inherent electrical conductivity. One of the promising methods to further activate MoS₂ is coupling engineering. Here, we demonstrate for the first time the synthesis of 2D MXene-MoS₂ nanocomposites through chemical vapor deposition (CVD) approach, thus leading to precise design in structure type and orientation. The computational results show that nanocomposites have metallic properties. Owing to their unique 2D/2D structure, MXene-MoS₂ nanocomposites exhibit more active catalytic sites, resulting in higher electrochemical performance, as inherited from parent excellent characteristics, and a much lower overpotential of ~ 69 mV at a current density of 10 mA·cm⁻² is achieved. This work paves the way to employ CVD method by coupling engineering to construct 2D nanocomposites for energy storage applications.