Indium selenide (InSe) is a novel narrow bandgap (1.3 eV) layered semiconductor with excellent plasticity and electrical properties, and has broad application prospects in new electronic and optoelectronic devices. Undoped and aluminum doped InSe crystals were grown by Bridgman method. The chemical composition and surface morphology of the prepared materials were characterized using energy dispersive spectroscopy (EDS) and scanning electron microscopy (SEM). This study founds that aluminum doping can regulate the plasticity and optoelectronic properties of InSe crystals. X-ray diffraction (XRD) analysis shows that the crystal has a hexagonal structure, and Raman spectroscopy characterization confirms that the crystal structure is ε-InSe. Nanoindentation measurements indicate that as the aluminum doping content increases, the hardness and modulus of InSe crystal decrease, while the plasticity of the material increases. Hall effect measurement and optical absorption spectrum results indicate that aluminum doping can increase the carrier concentration and bandgap width.