To measure the photocatalytic performance of N-doped TiO2-pillared clay nanocomposites (N-TiO2-PILC) for Cr(VI) removal under visible light, this paper prepares N-TiO2-PILC samples by sol-gel method and characterized them by scanning electron microscopy (SEM), X-ray diffraction (XRD), Brunauer–Emmett–Teller (BET) analysis and energy-dispersive X-ray spectroscopy (EDS). The author also explored the preparation conditions, settleability and reusability of the samples. The results show that N-TiO2-PILC had uniform pore size distribution, a large specific surface area (SSA) and an anatase crystal structure. The pillaring successfully introduces TiO2 particles into the clay, giving the composites a uniform interlayer structure. In addition, the optimal acid-base ratio and Ti/ clay ratio were determined as 3:1mL/mL and 15:1mmol/g, respectively; the optimal calcination temperature was proved to be 500 °C. The research findings shed new light on the removal of Cr(VI) in water under visible light.