The BixOyIz and CoFe2O4 combination enhances photocatalytic degradation of tetracyclines (TCs). Three TC antibiotics including TC, oxytetracycline (OTC), and chlortetracycline (CTC) with high concentration (50 mg L−1) were utilized as target pollutant. Bi5O7I/Bi4O5I2, with its Z‐scheme, improves removal efficiency to 1.6 times that of Bi5O7I and 1.4 times that of Bi4O5I2. Ternary Bi5O7I/Bi4O5I2/CoFe2O4 (I/I/Co) composites further increase efficiency, with I/I/Co‐2 achieving 1.6 times that of I/I‐2. The improved performance is due to an optimized microstructure, which promotes light absorption and carrier transfer. CoFe2O4 nanoparticles on nanosheets create a double‐Z band structure, enhancing redox activity. Radical trapping experiments indicated the major active species (•O2−, OH−, and h+) in photocatalytic process of I/I/Co‐2. Based on their enhanced removal efficiencies for high‐concentration TCs, proper magnetic separation capacity, and recycling performance, the practical applications of I/I/Co composites to treat real TC wastewater might be implemented.