Previous investigations on the Al2O3 barrier layer were only on TiO2 nanocrystalline electrodes or FTO electrodes. For instance, Palomares et al. showed a 2-2.5 nm Al2O3 barrier layer coated on TiO2 film resulted in a 4 fold retardation of the electron recombination with dye cations, and an efficiency of 5% was reached [30]. Another study by Liu et al. prepared a thin Al2O3- sheathed 3-dimentional (3-D) fluorinated tin oxide (FTO) as photoanodes of DSCs, at the aid of drift transport at the FTO/Al2O3 interfaces, an efficiency of 1.536% was obtained [7]. In addition, Gao et al. received improved photovoltaic performance made by using Al2O3 barrier layer coating on TiO2 nanotubes in conjunction with TiCl4 surface modification [31]. We have demonstrated FTO@TiO2 anode for DSCs with high efficiency at low dye loading levels [4]. Coating of Al2O3 barrier layer on F-T films is conducted to further increase the PCE by retarding the recombination processes. An efficiency of 5.24% is obtained.