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The combination of peroxymonosulfate (PMS) activation and photocatalysis has proven to be effective for organic contaminants treatment. However, the construction of an efficient catalytic material is an important challenge. Herein, novel Bi2WO6/BiOCl heterojunction nanocomposites were successfully designed and fabricated using a facile and effective strategy for bisphenol A (BPA) photodegradation with PMS activation. The well-designed heterojunction with improvement of the contact area and interface microstructure was obtained through in situ growth of the Bi2WO6 on the surface of BiOCl. The Bi2WO6/BiOCl nanocomposites exhibit excellent catalytic performance in PMS activation for BPA degradation under visible light irradiation. A possible photocatalytic reaction mechanism was systematically revealed. The excellent catalytic performance is mainly attributed to the strong interaction between Bi2WO6 and BiOCl, resulting in an enhanced photoabsorption and a more efficient interfacial charge separation and transfer. This paper provides a novel strategy to design efficient catalytic materials for organic contaminants remediation with PMS activation.