Image credit: UnsplashThe development of low-cost and high active electrocatalysts for hydrogen evolution reaction (HER) is essential for the sustainable energy and environment. Here we report a hydrothermal method to prepare ZnS@MoS2 nanosheets with hydrangea-like superstructure for enhanced HER. Benefiting from their abundant edge sites and facilitated charge transfer, the ZnS@MoS2 exhibited excellent HER performance with low overpotential of 106 mV and small Tafel slope of 73 mV dec−1. In addition, the chronoamperometry measurement results suggested the well-remained current density for 36 h without significant change, which indicated the excellent stability of ZnS@MoS2 superstructure. This work not only provides an effective method for constructing hierarchical heterojunctions, but also gives us a multi-scale strategy for the regulation of metal-based nanomaterials’ structure in energy-related applications.