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Photoelectrochemical (PEC) hydrogen generation is a promising solar energy harvesting technique to address the concerns about the ongoing energy crisis. Antimony selenide (Sb₂Se₃) with van der Waals‐bonded quasi‐1D (Q1D) nanoribbons, for instance, (Sb₄Se₆)_n, has attracted considerable interest as a light absorber with Earth‐abundant elements, suitable bandgap, and a desired sunlight absorption coefficient. By tuning its anisotropic growth behavior, it is possible to achieve Sb₂Se₃films with nanostructured morphologies that can improve the light absorption and photogenerated charge carrier separation, eventually boosting the PEC water‐splitting performance. Herein, high‐quality Sb₂Se₃films with nanorod (NR) array surface morphologies are synthesized by a low‐cost, high‐yield, and scalable close‐spaced sublimation technique. By sputtering a nonprecious and scalable crystalline molybdenum sulfide (MoS₂) film as a cocatalyst and a protective layer on Sb₂Se₃NR arrays, the fabricated core–shell structured MoS₂/Sb₂Se₃NR PEC devices can achieve a photocurrent density as high as −10 mA cm⁻²at 0 V_RHEin a buffered near‐neutral solution (pH 6.5) under a standard simulated air mass 1.5 solar illumination. The scalable manufacturing of nanostructured MoS₂/Sb₂Se₃NR array thin‐film photocathode electrodes for efficient PEC water splitting to generate solar fuel is demonstrated.