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Hydrogen gas (H₂) is being intensively proposed as a next-generation clean energy owing to the depletion of fossil fuels. Electrochemical water splitting is one of the most promising processes for hydrogen production. Furthermore, many efforts focusing on electrochemical water splitting have been made to develop low-cost, electrochemically active, and stable catalysts for efficient hydrogen production. MoS₂ has emerged as an attractive material for developing catalysts for the hydrogen evolution reaction (HER). Hence, in this study, we design hierarchically ordinated two-dimensional (2D) MoS₂ nanosheets on three-dimensional (3D) reduced graphene oxide (rGO) (H-2D/3D-MoS₂-rGO) aerogel structures as a new class of electrocatalysts for the HER. We use the one-pot hydrothermal synthesis route for developing high-performance electroactive materials for the HER. The as-prepared H-2D/3D-MoS₂-rGO contains a unique 3D hierarchical structure providing large surface areas owing to the 3D porous networks of rGO and more active sites owing to the many edge sites in the MoS₂ nanosheets. In addition, the H-2D/3D-MoS₂-rGO structure exhibits remarkable electrochemical properties during the HER. It shows a lower overpotential than pure MoS₂ and excellent electrochemical stability owing to the large number of active sites (highly exposed edge sites) and high electrical conductivity from the rGO structure.