lack of high-performance catalysts regardless of electrolyte pH. [7][8][9] Although optimizing the acidity of the electrolyte can tune the activity of a catalyst, designing the pseudo-pH-independent catalyst may make the water electrolyzers more affordable and safer for commercial H 2 production and home usage, respectively. [10,11] As one of the most renowned transitional metal dichalcogenides (TMDs), molybdenum disulfide (MoS 2 ) shows significant tuning potential for HER. [12][13][14][15][16][17] However, due to the inefficient cleavage of water molecules and sluggish H desorption, the activity of MoS 2 is unsatisfactory in overall pH values. [18][19][20][21][22] As reported by previous works, although the limited edge site with the unsaturated coordination is an active site for HER, especially in acidic media, the whole basal plane with the majority of atoms is immensely inert, the essence of the disappointing HER performance. [23][24][25] More specifically, the unsuitable orbital composition in the conduction band of MoS 2 , including S 3p x,y and Mo 4d z 2 , possesses an unfavorable electron-interaction with H atoms and water molecules on account of improper orbital orientation, rendering the basal plane of MoS 2 become inert for HER. [23,26] Several strategies, such as hetero-atom doping, [27][28][29][30][31] phase and interface tuning, [32,33] and defect engineering [34] have been employed to untangle the above drawback. For instance, Duan and co-workers synthesized the active basal plane of MoS 2 by replacing some Mo atoms with Co, which induces long-range ferromagnetic order to activate S atoms. [35] Moreover, Zheng and the colleagues prepared an active and stable catalyst via co-confining Se in the surface and Co in the inner layer of MoS 2 . [36] They proved that the activating effect of Co with the stabilizing effect of Se enables the formation of abundant active sites in the basal plane and the edges of MoS 2 . Previously, our research group fabricated carbon-induced MoS 2 via a controlled sulfurization of Mo 2 C. [26] Experimental and theoretical analyses revealed that carbon effectively altered the electronic and coordination structures of MoS 2 through emptying 2p orbitals perpendicular to the basal plane, enabling energetically favorable water adsorption and dissociation. Besides, Xiong et al. synthetized a bifunctional catalyst by doping Co atoms into the MoS 2 matrix. [37] They demonstrated that Co doping not only dramatically enhances HER performance but also induces superior MoS 2 represents a promising catalyst for the hydrogen evolution reaction (HER) in water splitting, but the inefficient catalytic activity in a pH-universal environment is an obstacle to developing practical applications. Boosting and balancing the water dissociation and hydrogen desorption kinetics is crucial in designing high-performance catalysts for the overall pH range. Herein, it is experimentally demonstrated that cobalt single-atom doping can effectively construct a reactive CoMoS micro-environment on the basal...