TiO2 nanoparticles (NPs) with a size of 240 nm (T240), used as a light-scattering layer, were applied on 25-nm-sized TiO2 NPs (T25) that were used as a dye-absorbing layer in the photoelectrodes of dye-sensitized solar cells (DSSCs). In addition, the incident light was concentrated via a condenser lens, and the effect of light concentration on the capacity of the light-scattering layer was systematically investigated. At the optimized focal length of the condenser lens, T25/T240 double layer (DL)-based DSSCs with the photoactive area of 0.36 cm2 were found to have the short circuit current (Isc) of 11.92 mA, the open circuit voltage (Voc) of 0.74 V, and power conversion efficiency (PCE) of approximately 4.11%, which is significantly improved when they were compared to the T25 single layer (SL)-based DSSCs without using a solar concentrator (the corresponding values were the Isc of 2.53 mA, the Voc of 0.69, and the PCE of 3.57%). Thus, the use of the optimized light harvesting structure in the photoelectrodes of DSSCs in conjunction with light concentration was found to significantly enhance the power output of DSSCs.