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In recent years, with the development of green environmental protection, starch film has become of interest due to the wide availability of sources, low price, and biodegradability. Amylose/polyvinyl alcohol (PVA) blend films crosslinked with different amounts of glutaraldehyde (GLU) were prepared by a solution casting method. The cross-linking degree, water sorption, tensile property, crystallization and section morphology of the films were examined. With the increase in glutaraldehyde concentration, the cross-linking degree of the blend film was improved. The wide-angle X-ray scattering (WAXS) result indicated that cross-linking hindered the crystallization of film. The section morphology of films was examined by scanning electron microscope (SEM). The results showed that the cross-linking degree of amylose film improved while the crystallinity decreased with the increase in glutaraldehyde content. Cross-linking had no obvious effect on the water sorption property of the blend films. The cross-linking modification significantly enhanced the tensile strength and Young’s modulus, while it reduced the elongation at break of the blend films. It was found that the film with 0.5 wt % glutaraldehyde possessed the best performance: the tensile strength increased by 115%, while the elongation at break decreased by 18% even at high relative humidity (RH) of 90% compared to non-crosslinked films. The developed amylose/PVA blend films have promising application prospects as agricultural mulch films and packaging materials.