Abstract
This study presents the development and analysis of hybrid polyurea composite materials. Neat polyurea was reinforced with cellulose nanocrystals (CNCs) and isocyanate-modified CNCs (CNC-ISOs) via a two-step prepolymer process. Introducing CNC considerably increased the mechanical strength and stiffness of the polyurea matrix. The tensile strength increased by up to 16.4%, and the Young modulus improved by approximately 29% compared to the pure polyurea. When CNC was functionalized with isocyanate, the interfacial bonding was further improved, and superior dispersion and load transfer were achieved. At 1.5% CNC-ISO loading, the modulus increased by approximately 128% compared to the unmodified matrix. Comprehensive analyses using FT-IR, XPS, DSC, TGA, DMA, tensile testing, and SEM showed that CNC-ISO films not only achieved higher tensile strength and better thermal stability but also formed a denser polymer network as evidenced by the increased crosslinking density. These findings highlight the importance of tailored nanofiller modification to create advanced polyurea composites with enhanced performance suitable for demanding protective and structural applications.