Most developed hydrogen evolution reaction (HER) electrocatalysts have pH-dependent functionalities, which limit their universal applications. Pt, the ideal HER electrocatalyst, is also highly effective in specific pH conditions. In the present article, we report a copper-based transition-metal chalcogenide from anion engineering. Hierarchical three-dimensional (3D) Cu 2 OÀ Cu 2 Se nanoflake arrays (COCS NFs) are grown directly on nickel foam (NF) by combining the rapid electrodeposition technique with the room temperature wet-chemical selenization method. Via the synergetic effects of the proper ratio of Se and O, as-synthesized COCS NFs manage to accomplish keyrequirements for pH-universal HER performances with overpotential values of 52.9, 62.8, and 77.8 mV, in alkaline, neutral, and acidic media, respectively, at 10 mA cm À 2 . The electrocatalyst also possesses superb stability at constant 10 mA cm À 2 current density for 50 h in all electrolytes. This work offers a synthesis protocol of a mixed-anion composite with the revelation about the importance of anion modulation towards electrode surface properties and HER performances.In recent years, different nanostructures and physical properties such as optical properties [9] and thermoelectricity [10] of transition-metal chalcogenides (TMCs) make them indispensable in various fields of research like energy conversion and storage, [11,12] dye-sensitized solar cells, [13] and photoelectrocatalysis. [14,15] Moreover, the inefficiency of energy-efficient electrodes in water electrolysis industry creates a potential market for highly efficient TMCs for electrocatalytic HER. [16,17] Recently, numerous TMCs, including CoS 2 , [18] CoSe x , [19,20] NiS 2 , [21] Ni 3 S 2 , [21] NiSe x , [22,23] SnSe 2 , [24] MoS 2 , [25] MoSe 2 , [26] WS 2 , [27] WSe 2 , [28] and ReSe 2 , [29] are studied for HER due to their low-cost and reasonable HER performances. However, individual metal sulfides or selenides as electrocatalysts exhibit nonideal electron transport and slow kinetics during HER because of their low electrical conductivities. More recently, Cu-based TMCs have garnered attention because of their abundant nature and low-cost. [30] For instance, Cu 2-x Se has an efficient HER activity in an acidic electrolyte, [31] but it is necessary to improve its HER performance in pH-universal electrolytes for commercialization. Recently published research works suggest that manipulation of the metal oxide surface is an useful direction for enhancing their HER performance because oxides such as NiO, [32] Co 3 O 4 , [33] Cu 2 O, [34] CeO 2 , [35] Mn 3 O 4 , [6] and TiO 2 [36] can participate in the reaction as water splitting promoters for HER. Although the use of Cu 2 O itself as a HER electrocatalyst is restrained due to its high overpotential and low current densities, the combination of Cu 2 Se with water dissociation promoters (Cu 2 O) by engineering the anion contents is expected to not only boost the HER kinetic but also optimize the free energy for hydrogen adsorption to achi...