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A novel series of the heterojunctions g‐CN/BBO(x) of g‐C3N4 (g‐CN) nanosheets decorated with spherical particles of BaBiO3 (BBO) were designed to enhance photocatalysis through interfacial charge transfer. The synthesized g‐CN/BBO(x) nanocomposites were characterized by various techniques such as XRD, FTIR, TEM, and SEM. Rhodamine B (RhB) dye and diclofenac sodium drug were taken as the model pollutants for the degradation under visible light. BBO facilitates the photocatalytic reaction after accepting electrons from the g‐CN. The g‐CN/BBO(30%) nanocomposite exhibits the best photocatalytic activity, which is 6.5 and 5 times higher than BBO and g‐CN, respectively. The enrichment in photodegradation is attributed to the combined effects of improved dye adsorption, visible light absorption, mobility of photogenerated carriers, and facial separation of electrons and holes (e−, h+) as supported by electrochemical impedance spectroscopy (EIS). This study provides new insight into the engineering, design, and stability of the g‐CN/BBO(x) heterojunction nanocomposite, as well as on its application and plausible mechanism for removal of harmful and detrimental pollutants such as RhB dye and diclofenac sodium drug under visible light. [ABSTRACT FROM AUTHOR]