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Though paper is an environmentally friendly alternative to plastic as a packaging material, it lacks antibacterial properties, and some papers have a low resistance to oil or water. In this study, a multifunctional paper-coating material was developed to reduce the use of plastic packaging and enhance paper performance. Natural cellulose nanocrystals (CNCs) with excellent properties were used as the base material for the coating. The CNCs were functionalized into dialdehyde CNCs (DACNCs) through periodate oxidation. The DACNCs were subsequently complexed using erythrosine as a photosensitizer to form an erythrosine–CNC composite (Ery-DACNCs) with photodynamic inactivation. The Ery-DACNCs achieved inactivations above 90% after 30 min of green light irradiation and above 85% after 60 min of white light irradiation (to simulate real-world lighting conditions), indicating photodynamic inactivation effects. The optimal parameters for a layer-by-layer dip coating of kraft paper with Ery-DACNCs were 4.5-wt% Ery-DACNCs and 15 coating layers. Compared to non-coated kraft paper and polyethylene-coated paper, the Ery-DACNC-coated paper exhibited enhanced mechanical properties (an increase of 28% in bursting strength). More than 90% of the bacteria were inactivated after 40 min of green light irradiation, and more than 80% were inactivated after 60 min of white light irradiation.