Recent progress in crystalline metal chalcogenides as efficient visible-light-driven photocatalysts for aqueous organic pollutant degradation is reviewed. Photodegradation of aqueous organic pollutants is a very promising strategy to address environmental issues and energy problems. Among all the reported photocatalysts, crystalline metal chalcogenides not only possess diverse architectures that can be enriched by integrating different metal ions and templates, but also have narrower band gaps (visible light adsorption) and suitable band positions that can be tuned through composition regulation. Therefore, the application of crystalline metal chalcogenides as efficient photocatalysts has attracted much attention. However, the limited synthetic methods, low degradation efficiency, and poor chemical stability are the major challenges that impede their practical application. In this review, the recent progress in employing crystalline metal chalcogenides as visible-light-driven catalysts for the photodegradation of organic contaminants is summarized. Besides this, the synthetic methods to prepare crystalline chalcogenides are discussed and the perspectives in regard to the improvement of the degradation efficiency and the chemical stability of metal chalcogenides are proposed.