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The concept of localized surface plasmon resonance has been applied to increase the absorption efficiency of dye-sensitive solar cells (DSSCs) by using various photoanode structures. A three-dimensional model for a photoanode of the DSSC based on composite materials was developed using COMSOL Multiphysics. Spherical-, rod- and triangular-shaped aluminum nanoparticles were employed in the core of SiO₂ to examine the influence of morphology on the performance of DSSCs in the 350–750 nm wavelength range. The UV-Vis absorption results indicated that aluminum nanoparticles with spherical, rod and triangle morphologies had 39.5%, 36.1% and 34.6% greater absorption capability than aluminum-free nanoparticles. In addition, we investigated the effect of plasmonic absorption in DSSCs for photoanodes made of TiO₂, SiO₂ and bilayer TiO₂/SiO₂ with and without covering aluminum nanoparticles. The TiO₂ and SiO₂ nanoparticles had fixed diameters of 90 nm each. The UV-Vis absorption and Tauc curves indicated that the TiO₂/SiO₂ bilayer structure (with and without aluminum nanoparticles) had greater absorption and lower bandgap energies than individual TiO₂ and SiO₂ nanoparticles. Furthermore, bilayer photoanode nanostructures were investigated based on nanospheres and nanorods for core–shell Al@SiO₂ nanoparticles. The results indicated that a photoanode with nanorod/nanosphere structure had a 12% better absorption capability than a nanosphere/nanorod configuration. This improvement in absorption is attributed to the high surface area, which boosts dye loading capacity and long-term light capture, resulting in greater interaction between the dye and the photon. Our study develops core–shell nanoparticles with optimized shape and materials for bilayer photoanode structures in photovoltaic technology.