Chitin (CT) and silk fibroin (SF) were selected as raw materials inspired by the chemical component of crustacean shell cuticle. The CT/SF biocomposite films were prepared by a facile casting method with the various CT/SF ratios and drying conditions (conventional and vacuum drying). The crystalline properties and the variation of other related characteristics for the biocomposite film were characterized by SEM, FTIR, UV-Vis, TG, XRD and electronic mechanical testing machine. The results show that as the ratio of m(CT):m(SF) varies from 1:4 to 4:1, the crystal appearance of the CT/SF biocomposite film gradually transforms from a loose 'radial dotted line' to a dense 'filiform net' under the conventional drying, while from "snow flower-like" to "worm-like" and then to "dotted line" under the vacuum drying. The drying condition plays a significant role on the variation of micro-morphology of the crystals of the biocomposite film when the ratio of m(CT):m(SF) is 4:1, changing from the 'scaly layer' under the conventional drying to the 'cactus ball' under the vacuum drying. Meanwhile, some microcrystals with a diameter of about 60 nm appear in the biocomposite film without crystallization at the same ratio. The biocomposite film with a m(CT):m(SF) ratio of 1:4 under the conventional drying exhibits the highest average transmittance (97.3%) when the wavelength of visible light is beyond 500 nm.The non-crystalline biocomposite film with the m(CT):m(SF) ratio of 4:1 under the vacuum drying shows the optimum comprehensive mechanical properties and thermal stability, corresponding to the tensile strength and elongation at break of 1.28 MPa and 134%, respectively. © 2022, Materials Review Magazine. All right reserved.