Estimates suggest that one-third of all food produced in the world is wasted. Besides generating economic costs, this is a huge burden on the environment. With related issues of nearly depleted landfill sites, food insecurity, and environmental degradation, there is an urgent need to create loops in food systems and ensure products are used to their full potential before ending up in landfills or incinerators. As untapped sources of cellulose, many of the major agricultural and food processing waste streams could offer a strategic opportunity to turn left-over residues into valuable nanocellulose materials. Here, we explore cellulose nanofibers (CNF) extracted from food waste as spray-coating solutions to replace plastic packaging that wraps fruits and vegetables in grocery stores. In the first step of our research, we investigate the use of carrot pomace from both fresh and stale carrots, apple peels, and broccoli (unsellable for retail) to produce CNF. The use of a one-pot bleaching pretreatment of the vegetable pulps along with the resulting CNF fiber morphology and quality (surface area, degree of polymerization, carbohydrate content) are analyzed. In addition, model films are prepared via vacuum filtration and hot-pressing, whereby film quality, as related to morphological, optical, mechanical, and barrier properties, is assessed. Finally, CNF suspensions are sprayed onto the surface of bananas and cucumbers, demonstrating a substantial delay in enzymatic browning and discoloration. Afterward, we investigate the addition of natural compounds such as carvacrol and ε-Poly-L-Lysine (εPL), as additives to CNF spray coating formulations to improve their protection behavior once applied onto fruit and vegetable surfaces. To achieve this goal, composite mixtures based on CNF and carvacrol via stabilizing octenyl-succinic anhydride (OSA)-modified epsilon polylysine (MɛPL-CNF) were prepared. The effects of εPL concentration and modification with OSA and carvacrol were evaluated concerning film morphology and mechanical, optical, antioxidant, and antimicrobial properties. Overall, our results suggested the potential of such waste-derived CNF materials to be used as biobased protective coatings for fruits and vegetables.