Surface sol-gel process conducted under mild experimental conditions was further used to deposit a conformal ultrathin layer of Al2O3 on F-T photoanodes, with the aim to modulate interfacial electron transfer dynamics and thereby improve the performance of DSCs combined with enhanced electron extraction of F-T film, A power conversion efficiency of 5.24% is obtained, improving by 12.4% of the solar cell based on bare F-T electrodes.