Free cyanide is a highly dangerous compound for health and the environment, so treatment of cyanide-contaminated water is extremely important. In the present study, TiO2, La/TiO2, Ce/TiO2, and Eu/TiO2 nanoparticles were synthesized to assess their ability to remove free cyanide from aqueous solutions. Nanoparticles synthesized through the sol–gel method were characterized by X-ray powder diffractometry (XRD), scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDS), Fourier-transformed infrared spectroscopy (FTIR), diffuse reflectance spectroscopy (DRS), and specific surface area (SSA). Langmuir and Freundlich isotherm models were utilized to fit the adsorption equilibrium experimental data, and pseudo-first-order, pseudo-second-order, and intraparticle diffusion models were used to fit the adsorption kinetics experimental data. Cyanide photodegradation and the effect of reactive oxygen species (ROS) on the photocatalytic process were investigated under simulated solar light. Finally, reuse of the nanoparticles in five consecutive treatment cycles was determined. The results showed that La/TiO2 has the highest percentage of cyanide removal (98%), followed by Ce/TiO2 (92%), Eu/TiO2 (90%), and TiO2 (88%). From these results, it is suggested that La, Ce, and Eu dopants can improve the properties of TiO2 as well as its ability to remove cyanide species from aqueous solutions.