The electroreduction of water for sustainable hydrogen production is an important process for clean energy technologies, such as water splitting and fuel cells. However, development of low-cost and efficient electrocatalysts for hydrogen evolution reaction (HER) is still a great challenge. Here we reported a kind of ultrathin chain-structured CuCo₂O₄ (CCO) and sulfured CuCo₂O₄ (S-CCO) for HER with excellent activity and good durability in alkaline solution. At a current density of 10 mA cm⁻², S-CCO nanocomposite catalyst only need an overpotential of 154 mV (vs. RHE), whereas chain-structured CCO need an overpotential of 490 mV. It demonstrates that sulfured treatment is an effective approach to enhance the catalytic activity of oxide for HER.