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This review delves into environmentally conscious sustainable packaging materials, focusing on biodegradable polymers and innovative surface modification methodologies. Synthetic plastics have revolutionized various industries due to their physical attributes and affordability, particularly in packaging applications. Nonetheless, the substantial volume of plastic waste, especially from non-biodegradable sources, has provoked heightened environmental apprehensions. Notably, polymers derived from natural sources, such as cellulose, are classified as biopolymers and esteemed for their ecological benevolence. Among these, cellulose and its derivatives stand out as renewable and abundant substances, holding promise for sustainable packaging solutions. Nano-sized cellulose fibers’ incorporation into biodegradable films garners interest due to their remarkable surface area, robust mechanical strength, and other commendable properties. Surface modification techniques, such as a polydopamine (PDA) coating, have been explored to improve the dispersion, interfacial compatibility, and mechanical performance of cellulose nanocrystals (CNC) when incorporated into biodegradable polymer films. In this sense, PDA, derived from mussel proteins’ dopamine component, displays exceptional adhesion to diverse surfaces and has been extensively scrutinized for its distinctive attributes. Therefore, the core focus of this review was to approach ecologically friendly packaging materials, specifically investigating the synergy between CNC and PDA. The unparalleled adhesive characteristics of PDA serve as a catalyst for enhancing CNC, thereby elevating the performance of biodegradable polymers with potential implications across various domains.