TiO2 pillared montmorillonite (PILM) was synthesized by hydrolyzing TiO2 Sol into the interlayers of montmorillonite (MMT) at low temperatures. It is novel that all the as-prepared catalysts without calcination show a high photocatalytic activity for the degradation of acid red G (ARG) under UV light irradiation. The as-prepared powders were characterized by XRD, TEM, UV-vis diffuse reflectance spectroscopy, BET, and FIF-IR. The X-ray diffraction analysis indicated that the (001) plane of MMT in the composites disappeared and that the layered structure became disordered, which also was confirmed by the TEM photographs. The UV absorption edge of the composites shows a red-shift in comparison to that of pure TiO2 particles. The obtained catalyst has the highest photocatalytic activity when the composite temperature is 70 degrees C, which could be attributed to the synergetic effects of the adsorbability of MMT and the photocatalytic property of TiO2 in it.