Exploring cost-effective and highly active photocatalysts is crucial for achieving the thorough breakdown of pollutants and addressing the inherent drawbacks of current photocatalytic technologies. In this research, a chrysanthemum-like Bi/BiOClBr photocatalyst was obtained for the first time using a straightforward solvothermal means. Various analytical methods were utilized to comprehensively analyze the characteristics of the composite materials. The exceptional photocatalytic effectiveness of Bi/BiOClBr was demonstrated by its efficient removal of pollutants such as rhodamine (RhB), tetracycline (TC) and ofloxacin (OFX). The presence of BiOCl and BiOBr heterostructures facilitated the movement of photogenerated carriers. Moreover, by incorporating metallic Bi into the composite, which manifests a surface plasmon resonance (SPR) effect, we not only notably augmented the composite's ability to absorb visible light but also functioned as an “electron trap,” thereby enhancing the efficiency of separating and transferring photogenerated electrons and holes. This work offered innovative perspectives in the development and fabrication of noble metal-free, decorated semiconductor photocatalysts with outstanding activity and reusability.