Al‐doped CuInSe2 material is prepared by a low‐cost wet chemical process. The key properties of Al‐doped CuInSe2 as a successful solar cell material are investigated, such as crystal structure, morphology, optical properties, and bandgap. In situ X‐ray diffraction measurements indicate that the doping of Al has induced noticeable lattice distortion. The material shows excellent thermal stability up to 600 °C annealing temperature. By increasing the Al‐doping concentration, the crystal unit‐cell parameter of the material becomes smaller and the change of crystal structure leads to an increase of the grain size and surface roughness. The bandgap of Al‐doped CuInSe2 can be continuously tuned in a range of 1.07–1.67 eV as Al/(Al + In) content ratio varies from 0 to 0.49. Finally, the effect mechanism on the properties of CuInSe2 after Al doping is discussed based on the ionic radius, crystal structure, and bonding state.