Organic pollutant is an environmentally harmful and ubiquitous aquatic pollutant with extensive production and application. In this study, a unique novel TiO2-based dual-sensitized heterojunction photocatalyst (PbS/CdS/TiO2) was successfully obtained by one step hydrothermal method, chemical bath deposition (CBD) method and ionic layer adsorption and reaction (SILAR) method. Scanning electron microscopy, X-ray photoelectron spectroscopy, transmission electron microscopy and energy dispersive spectrometer characterized the composition. PbS/CdS was successfully decorated on the surface of TiO2 nanosheet array. As a stable catalyst with wide-spectrum (300–800 nm) optical response, excited electron–hole pairs of PbS/CdS/TiO2 could apply in degrading organic pollutants. Successfully, the degradation efficiency of PbS(5 C)/CdS(30 min)/TiO2 nanocomposites reached 99.9% under visible light, which was 5 times over pure TiO2. This ternary heterostructured materials will be well-promising photocatalysts.