The aim of this work was to demonstrate the production potential of a combination of the two materials cellulose nanofibrils (CNF) and chitin nanowhisker (CNW) using wheat straw and chitin. CNF and CNW were prepared from TEMPO-oxidation and acid hydrolysis prior to high-pressure homogenization. The zeta potential results indicated the differences in the suspended mechanism for the CNF and CNW dispersions. Fourier transform infrared spectroscopy (FTIR) and X-ray diffraction (XRD) revealed that the chemical composition and crystal unit changes during the chemical separation process. Hybrid CNF/CNW films were prepared via casting and evaporation. The films had better mechanical properties, which were ascribed to multivalent physical interactions between CNF and CNW. However, increasing the CNW content up to 50% negatively affected the mechanical properties of the hybrid films. In addition, all films showed high transparency and excellent flexibility. These results indicated that the interaction between CNF and CNW effectively enhanced the mechanical performance of films.