Smart packaging can provide real-time information about changes in food quality and impart a protective effect to the food product by using active agents. This study aimed to develop a smart bilayer film (alginate/agar) with a cellulose nanosphere (CNs) from corncob. The bilayer films were prepared using 1.5% (w/w) sodium alginate with 0.25%% (w/v) butterfly pea extract incorporated (indicator layer) and 2% (w/w) agar containing 0.5% (w/v) catechin–lysozyme (ratio 1:1) (active layer). The CNs were incorporated into the alginate layer at different concentrations (0, 5, 10, 20, and 30% w/w-based film) in order to improve the film’s properties. The thickness of smart bilayer film dramatically increased with the increase of CNs concentration. The inclusion of CNs reduced the transparency and elongation at break of the smart bilayer film while increasing its tensile strength (p < 0.05). The integration of CNs did not significantly affect the solubility and water vapor permeability of the smart bilayer film (p > 0.05). The smart bilayer film displayed a blue film with a glossy (without CNs) or matte surface (with CNs). The developed bilayer film shows excellent pH sensitivity, changing color at a wide range of pHs, and has a good response to ammonia and acetic acid gases. The film possesses exceptional antimicrobial and antioxidant activities. The integration of CNs did not influence the antibacterial activity of the film, despite the presence of a higher level of DPPH in film containing CNs. The smart bilayer film was effectively used to monitor shrimp freshness. These findings imply that smart bilayer films with and without CNs facilitate food safety and increase food shelf life by monitoring food quality.