Cellulose nanocrystals (CNCs) were extracted from orange peels using an alkaline/H₂O₂ bleaching pre-treatment followed by sulfuric acid hydrolysis. Extracted CNCs were added as reinforcing agent into films based on chitosan/hydroxypropyl methylcellulose blend (CS/HPMC) enriched with lauroyl arginate ethyl (LAE) to produce bio nanocomposite active films. The size and morphology of CNCs were characterized by transmission electron microscopy. In addition, the effect of CNCs (10% w/w of biopolymer) and LAE (5% w/w of biopolymer) on microstructural, optical, mechanical, water barrier, and antimicrobial properties of the CS/HPMC films were analyzed. CNCs displayed needle-like shapes morphology with an average length of 500 nm, an average width of 40 nm. Scanning electron microscopy illustrated structural integrity and compatibility between CS/HPMC/CNCs and incorporated LAE. The successful incorporation of CNCs and LAE was confirmed by fourier transform infrared spectroscopy mainly due to the formation of hydrogen linkages between film matrix and incorporated CNCs and LAE. This nanocomposite active film showed improvement in UV-Vis light barrier properties (p<0.05). The addition of CNCs to CS/HPMC caused a reduction in water vapor permeability, while tensile strength was improved due to the homogeneous distribution of the nanoparticles within the polymer matrix. On contrary, LAE incorporation into CS/HPMC improved the elasticity and also caused antimicrobial activity against S. enterica subsp. Thyphimurium and L. monocytogenes. Overall, nanocomposite films based on CS/HPMC/CNCs enriched with LAE could represent a suitable green approach for a partial replacement of synthetic plastics for packaging foods sensitive to microbiological decay and spread of foodborne pathogens.