Starch-based biodegradable films were prepared by using solution-casting method and reinforced by agricultural residues [apricot and walnut shell (APS and WNS) powder]. The powder of both shells was added in different ratios (0, 2.5, 5, 7.5, and 10%) to investigate the microstructures and performances (mechanical and thermal properties) of the starch-based film. Different techniques such as impact, tensile testing, scanning electron microscope, optical microscope (OM), X-ray diffraction (XRD), water vapor transmission rate (WVTR), and dynamic mechanical analysis were applied to study the thermomechanical and barrier properties of the composite films. Results showed that the incorporation of both shells significantly improved the WVTR and mechanical properties of starch-based films. The shells powder was significantly increased the Young's modulus and tensile strength of the starch-based films. Both OM and SEM results showed reasonably good compatibility between starch and reinforced shells. OM and XRD indicated that the APS and WNS not only retained their crystalline structure in the film but they also strengthened the peak intensity of the film. This phenomenon can be used to explain the mechanism of mechanical reinforcement. Since all the components used in the preparation of the films are food grade ingredients, it is expected that the films developed in this work will be used for food packaging applications.