The mechanical properties and miscibility of polymer‐based composites containing cellulose nanofiber (CNF) and polyrotaxane (p‐rtx) as organic fillers were studied in detail. CNF and p‐rtx were introduced as powders into a polypropylene (PP) matrix, and composites were prepared using a simple melt‐compounding method. The best mechanical properties were achieved when CNF and p‐rtx were loaded at a concentration of 0.6 wt%. The Young's modulus of the composite increased by 760 MPa compared with that of the PP matrix. In addition, the presence of mica in the composite promoted the epitaxial growth of PP along the (1 3 0) plane. The various shifts in the melting/crystallization temperatures of the composites prepared at different CNF:p‐rtx ratios confirmed the partial miscibility between the fillers and the matrix. The enhancement in the mechanical properties of the composite is believed to be due to the miscibility of the surfaces of aggregates of the organic fillers with PP and the uniform dispersion of the organic fillers in the matrix.
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