This work demonstrates Al-doped ZnO adsorbents successfully synthesized by glucose-assisted solution combustion. The addition of glucose results in nanocomposite powders with highly fluffy network, mesoporous structure, high specific surface area, and physical properties, which in turn improve the adsorption properties. The adsorption performance of the material was studied, and the influence of Al doping concentration, adsorbents and methyl orange concentration in the solution were investigated. The addition of glucose increased the adsorption capacity of methyl orange onto Al-doped ZnO by over 2 times. The adsorption followed the Langmuir isotherm, was spontaneous and exothermic. Kinetic calculations show that the adsorption followed the pseudo-second-order model with a multistep diffusion process. Thermodynamic parameters indicate that the adsorption is a feasible, spontaneous, and exothermic process.