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Integrating solar energy into rechargeable battery systems represents a significant advancement towards sustainable energy storage solutions. Herein, we propose a win‐win solution to reduce the shuttle effect of polysulfide and improve the photocorrosion stability of CdS, thereby enhancing the energy conversion efficiency of rGO/CdS‐based photorechargeable integrated lithium‐sulfur batteries (PRLSBs). Experimental results show that CdS can effectively anchor polysulfide under sunlight irradiation for 20 minutes. Under a high current density (1 C), the discharge‐specific capacity of the PRLSBs increased to 971.30 mAh g−1, which is 113.3 % enhancement compared to that of under dark condition (857.49 mAh g−1). Remarkably, without an electrical power supply, the PRLSBs can maintain a 21 hours discharge process following merely 1.5 hours of light irradiation, achieving a breakthrough solar‐to‐electrical energy conversion efficiency of up to 5.04 %. Ex situ X‐ray photoelectron spectroscopy (XPS) and in situ Raman analysis corroborate the effectiveness of this complementary weakness approach in bolstering redox kinetics and curtailing polysulfide dissolution in PRLSBs. This work showcases a feasible strategy to develop PRLSBs with potential dual‐functional metal sulfide photoelectrodes, which will be of great interest in future‐oriented off‐grid photocell systems. [ABSTRACT FROM AUTHOR]

The rational design and construction of cost‐effective nickel‐based phosphide or sulfide (photo)electrocatalysts for hydrogen production from water splitting has sparked a huge investigation surge in recent years. Whereas, nickel phosphides (NixPy) possess more than ten stoichiometric compositions with different crystalline. Constructing NixPy with well crystalline and revealing their intrinsic catalytic mechanism at atomic/molecular levels remains a great challenge. Herein, an easy‐to‐follow phase‐controllable phosphating strategy is first proposed to prepare well crystalline NixPy (Ni3P and Ni12P5) modified CdS@Ni3S2 heterojunction electrocatalysts. It is found that Ni3P modified CdS@Ni3S2 (CdS@Ni3S2/Ni3P) exhibits remarkable stability and bifunctional electrocatalytic activities in both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Density functional theory results suggest that P–Ni sites and P sites in CdS@Ni3S2/Ni3P, respectively, serve as OER and HER active sites during electrocatalytic water splitting processes. Moreover, benefiting from the advantageous photocatalyst@electrocatalyst core@shell structure, CdS@Ni3S2/Ni3P delivers an advantaged photoassisted electrocatalytic water splitting property. The champion electrical to hydrogen and solar to hydrogen energy conversion efficiencies of CdS@Ni3S2/Ni3P, respectively, reach 93.35% and 4.65%. This work will provide a general guidance for synergistically using solar energy and electric energy for large‐scale H2 production from water splitting. [ABSTRACT FROM AUTHOR]