Plant protein films are a research hotpot in the current food packaging field for their renewable and bio-compatibility, and further improving the physicochemical properties of plant protein films in combination with biodegradable materials is of great significance. In this study, we selected cellulose nanocrystals (CNC) to modify the protein films with soybean protein isolate (SPI), wheat gluten protein (WGP), and Zein, and the physicochemical properties were studied. The results showed that the hardness and opacity of Zein-based films decreased by 16.61% and 54.12% with the incorporation of CNC, respectively. The SPI-based films performed with lower hardness and higher tensile strength. The thickness and opacity of WGP-based films increased by 39.76% and 214.38% after combination with CNC, respectively. Accordingly, this study showed that CNC could largely modify the physicochemical properties of the plant protein films, which provided a reference for the preparation of modified plant protein films using biodegradable materials.