Abstract Sisal fiber‐reinforced thermoplastic starch (TPS) composites with excellent properties have been widely used in agriculture, packaging, and other fields. In this work, a new type of sisal/starch composite was prepared by torque rheologic melting and a hot pressing process successively, improving the compatibility between sisal fibers and TPS. The additives of glutaraldehyde and starch nanocrystals played an important role in improving the properties of the composites. They not only improved their surface smoothness, uniformity, compatibility, and interfacial adhesion strength but also promoted the mechanical properties that was because the interaction between the matrix and fibers was formed to effectively promote stress dispersion and share the load to enhance the deformation ability. These additives also promoted the cross‐linking function of the composites and reduced the number of hydroxyl groups on their surface, decreasing the moisture absorption rate. After cross‐linking with these compatibilizers, the hydrophobicity of the composites improved, decreasing their water vapor permeability.
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