AbstractSpray‐dried cellulose nanocrystal (SDCNC) particles have attracted intense interest as reinforcements in polymer composites because of their unique physical and mechanical properties. This work aims to develop homopolymer polypropylene (HPP) composites with different loading levels of SDCNC particles (5, 10, 15, and 30 wt%) to understand their impact on composite mechanical, morphological, and thermal properties. The SDCNC‐reinforced HPP composites were manufactured using a C.W. Brabender bowl internal mixer with a masterbatch concept and an injection molding process. The mechanical, morphological, and thermal properties of the composites were investigated. Compared to pure HPP, the tensile, and flexural modulus of elasticity (MOE) of composites with 30 wt% SDCNC significantly increased by up to 67% and 49%. The impact strength of the composites with the absence of a compatibilizer significantly increased by up to 19%, which was attributed to the mechanical interlocking network established between SDCNC particles and HPP. Additionally, increasing SDCNC loading in the composites led to higher crystallization peak temperatures and increased the degree of crystallinity (especially at 30 wt% SDCNC content), indicating that the SDCNC particles can act as heterogeneous nucleating agents during the crystallization process. The thermal stability of the composite was slightly improved upon SDCNC introduction.Highlights With the incorporation of spray‐dried cellulose nanocrystal (SDCNC), the tensile modulus of elasticity (MOE), flexural MOE, and impact strength of filled homopolymer polypropylene (HPP) composites were significantly improved by up to 67%, 49%, and 19%, respectively. Mechanical interlocking network established between SDCNC and HPP contributed to the enhanced the impact strength. SDCNC particles can act as heterogeneous nucleating agents to promote the crystallization process of HPP. SDCNC particles slightly enhanced the thermal stability of HPP composite.
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