An efficient visible-light active photocatalyst of porous CrOx–Ti1.83O4 nanohybrid with a 1:1 type ordered heterostructure is synthesized through a hybridization between a chromia cluster and exfoliated titanate nanosheets. The present nanohybrids are found to have a large surface area (ca. 250–310 m2 g–1) and an intense absorption of visible light, ascribable, respectively, to the formation of a porous structure and the hybridization of titanate with narrow-bandgap chromium oxide. After the calcination at 400 °C, the nanohybrid shows an enhanced photocatalytic activity to effectively decompose organic compounds under the irradiation of visible light (λ > 420 nm). The present study highlights the exfoliation–restacking route as a very powerful way to develop efficient visible-light-harvesting photocatalysts with excellent thermal stability.