A bismuth oxyiodide (BiOI) photocatalyst with excellent sunlight-driven performance was synthesized by a solvothermal route without the addition of surfactants or capping agents. The prepared photocatalyst exhibited a tetragonal phase with an energy band gap of 2.15 eV. The efficiency of the photocatalyst was elucidated by monitoring the photodegradation of organic dyes and antibiotics. The BiOI photocatalyst provided a 95% removal of norfloxacin (NOR) antibiotics under visible light illumination. Interestingly, the complete removal of Rhodamine B (RhB) dye was achieved after 80 min of natural sunlight irradiation. The photodegradation reaction followed the first-order reaction. Both photo-generated holes and electrons play vital roles in the photodegradation of the pollutant. The BiOI photocatalyst remains stable and still shows a high efficiency even after the fifth run. This confirms the great cycling ability and high structural stability of the photocatalyst. The prepared BiOI catalyst, with a high surface area of 118 m2 g−1, can act as an excellent adsorbent as well. The synergistic effect based on both adsorption and photocatalysis is a key factor in achieving a very high removal efficiency. The photoactivity under sunlight is higher than that observed under visible light, supporting the practical use of the BiOI photocatalyst for the removal of organic pollutants in wastewater through the utilization of abundant solar energy.