Low-temperature, solution-processed, highly efficient hybrid organic/inorganic perovskite planar heterojunction solar cells were fabricated by incorporating reactive crystalline titania (h-TAc) into MAPbI3 layers. The h-TAc was prepared by the sol-gel reaction at low temperature followed by solvothermal treatment. The photoelectrical properties of the solar cells with h-TAc were analyzed. The incorporation with 0.85-wt% h-TAc showed the highest power conversion efficiency (PCE, 15.9%), increasing 69% compared to the pristine cell. The enhancement arose from large-grained microstructures, leading to a low rate of charge recombination. The carboxyl groups chelated on the surface of h-TAc revealed a strong attraction to lead ions, which are significantly helpful to MAPbI3 crystal growth.