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Natural source-based composites became promising substitutes and synthetic petrochemical-based counterparts. So far, thermoplastic starch and lignocellulosic fibers are the most common materials for making such eco-friendly "green" materials. Low cost, abundance, and renewability are the factors that lead to deploying these two types of materials. In this chapter, we are conducting further analysis for previously published results of six types of high-content natural fiber-reinforced starch-based composites. All composites were prepared by compression molding under pressure from 5 to 20 MPa and temperature from 130 to 160°C. Composites exhibited highest tensile strength and modulus of elasticity at fiber weight content from 50 to 70%, and then mechanical properties deteriorated significantly at 80% fiber content due to the insufficient starch resin. For instance, the tensile strength was boosted up from 2-12 MPa for thermoplastic starch to reach 55,45,32,28,44, 365 MPa for flax, bagasse, date palm fiber (DPF), banana, bamboo, and hemp composites, when fiber content was increased from 0% to the optimum fiber content (50-70%). Kelly-Tyson (random 2d) was the optimum model to predict random fiber composite. Increasing the fiber content and choosing a fiber with high cellulose content significantly improve the moisture resistance of the composites. Fick's law of diffusion predicted the water uptake property successfully. The thermal stability of composites was improved with increasing the fiber weight content as well. This is attributed to the high thermal stability of cellulose when compared to starch. Properties exhibited by starch-based high-content natural fiber composite are promising for many industrial and biomedical applications.