Realizing the efficient treatment of acid drainage using semiconductor photocatalysis at low pH values remains a challenging and necessary project for widespread heavy metal ions and organic aromatic pollutants. Here, the synergistic photocatalytic remediation of hexavalent chromium and phenol under visible light was studied with the purpose of both environmental remediation and sustainable development in mind. Using a structural engineering strategy, the typical CdS-based heterojunction with outer nanocrystal cluster protection is un-precedentedly endowed with the efficient and recyclable capability of a visible-light-driven photocatalysis for the remediation of pollutants in strong acidic conditions. Owing to the structure-enabled acidic stability, the simultaneous remediation of Cr(VI) and phenol can be undertaken in an efficient and recyclable mode at pH = 2.0-7.0. This study fundamentally evolves a representative photocatalytic system into one with more industrial and practical applications foracid drainage purification.