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Antimony selenide (Sb2Se3) has developed as an eco‐friendly photovoltaic candidate owing to its non‐toxic composition and exceptional optoelectronic properties. However, the toxic and parasitic light‐absorbing CdS are widely used as electron transport layer (ETL) in Sb2Se3 solar cells, which severely limits its development. Herein, an alternative, zinc tin oxide (ZTO) ETL with varying composition‐dependent energy structure is deposited by atomic layer deposition (ALD) technique and used for constructing Cd‐free Sb2Se3 solar cells. It has been found that the ZTO ETL possessing an appropriate Zn/Sn ratio can alter the Sb2Se3/ZTO heterojunction band alignment to an ideal “spike‐like” arrangement. It not only suppresses the accumulation and recombination of charge carriers at the interface, but also effectively enhances carrier transport. In addition, thanks to the formation of passivated Sb2O3 ultra‐thin layer upon ALD process, the non‐radiative recombination within bulk Sb2Se3 can be effectively suppressed, and therefore enhancing carrier lifetime, extraction efficiency, and collection efficiency. Consequently, the as‐fabricated Mo/Sb2Se3/ZTO/ITO/Ag thin‐film solar cell demonstrates an impressive efficiency of 8.63%. This accomplishment establishes it as the most efficient Cd‐free Sb2Se3 solar cell to date, underscoring the significant advantages of incorporating ZTO ETL in the development of Sb2Se3 photovoltaic scenarios. [ABSTRACT FROM AUTHOR]