TiO₂ is a catalyst that can effectively degrade organic pollutants with the following advantages, low cost, simplicity, and pollution-free nature. In recent years, the non-noble plasmonic metal Al has effectively improved the photocatalytic performance of TiO₂. However, the current reports are limited to the photocatalytic performance of Al/TiO₂ on the substrate, which requires expensive large-scale vacuum equipment. In this study, monodispersed Al particles were proposed to enhance the photocatalysis of TiO₂. The localized surface plasmon resonance (LSPR) effect of Al is proven by finite difference time domain method (FDTF) simulation. Then, Al/TiO₂ composites were prepared by combining monodispersed Al and TiO₂. The influence of ligand (glutathione (GSH), glutamic acid (GAG), or 3-mercaptopropane acid (MPA)), Al size (40 to 300 nm), and the ratio of Al to TiO₂ (0.5:1 to 10:1) on the photocatalytic degradation of methylene blue (MB) by Al/TiO₂ were discussed. The obtained results showed that the Al/TiO₂ composite which were prepared with 200 nm Al particles, GSH as the ligand bridge, and an Al:TiO₂ ratio of 1:1 had the best MB degradation effect. It can degrade 97.7% of 10 mg/L MB in 100 min. The reaction rate of the Al/TiO₂ composite with the optimal photocatalytic performance is k=3.36×10^-2 min^-1, which is 10 times that of P25 TiO₂. In addition, Al/TiO₂ has a good photocatalytic effect on rhodamine B (RhB) and crystal violet (CV). Therefore, Al/TiO₂ composites with the advantage of high efficiency are a type of potential photocatalytic material that can be used for the photocatalytic treatment of organic pollutants in water.