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TiO2 nanoblets coated with MoS2 nanosheets, donated as T@M, were successfully prepared by a facile hydrothermal method. In comparison with pristine TiO2 nanoblets, the composite of MoS2 nanosheets could enlarge the spectral response of sunlight. The surface heterostructures of T@M nanocomposite could effectively separate the photogenerated electron‐hole pairs, and greatly inhibit the recombination of photogenerated electrons and holes. The photocatalytic performances of the as‐synthesized products were investigated in contrast by photodegradation of methylene blue, methyl orange, rhodamine B and levofloxacin. Under 350 W Xe lamp irradiating for 2 h, T@M exhibited excellent degradation performance. Interestingly, blue shifts of the dyes’ absorption peaks were observed, which probably attributed to the incomplete products decomposed by as‐absorbed dye molecules on the surface of TiO2 nanoblets. Compared with pure TiO2 nanoblets, T@M has less amount TiO2, higher separation efficiency of photogenerated electron‐hole pairs and better inhibition efficiency of photogenerated carriers’ recombination, leading less blue shift and higher degradation efficiency.