The food industry is considered one of the main contributors to plastic waste due to packaging. Sustainable and degradable packaging solutions are the need of the hour. Biopolymers have proved to be a promising replacement for petroleum-based polymers. The main reason is their various intrinsic properties, such as antimicrobial nature and degradability. The main objective of this study was to develop chitosan/nanocrystalline cellulose- and polylactic acid-based biofilms. The biofilms were developed using the drop-casting method. The developed biofilms were characterized by scanning electron microscopy, Fourier transform infrared spectroscopy, X-ray diffraction, differential scanning calorimetry and thermogravimetric analysis. The performance of the biofilms was checked using mechanical, water solubility, porosity, antioxidant and antibacterial activity tests. The developed biofilms can solve the issues of environmental pollution being faced by the food packaging industry.