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Perovskite oxides, renowned for their adaptable structure and optoelectronic characteristics, hold significant potential for applications in catalysis and photoelectrochemical (PEC) processes. In this research, the preparation of praseodymium iron oxide (PrFeO3) by spin coating and the impact of incorporating a calcium (Ca) dopant on its PEC efficacy as photocathodes are investigated. Spin coating of a polymer containing sol–gel yields thin films with uniform morphology and porosity, facilitating effective semiconductor/electrolyte interactions, as characterized by scanning electron microscopy analyses. Evaluation of transient photocurrent responses reveals that introducing Ca at a 5 at% doping level significantly enhances the PEC activity of PrFeO3, resulting in an optimal photocurrent of −124 μA cm−2 at +0.43 V vs. a reversible hydrogen electrode (VRHE) under simulated sunlight conditions. This enhancement is accompanied by an incident photon‐to‐current efficiency (IPCE) of 3.8% at +0.43 VRHE and 350 nm, along with an onset potential of +1.1 VRHE. Ultraviolet and visible spectroscopy analyses indicate an increase in light‐absorption capabilities in the Ca‐doped films and a noticeable reduction in bandgap compared to the undoped counterparts, further supported by IPCE measurements. In the findings, the significant role of dopants in augmenting the photocurrent performance of stable perovskite oxides, highlighting their potential in advancing photon conversion technologies, is underscored. [ABSTRACT FROM AUTHOR]