Cellulose possesses numerous favorable peculiarities to replace petroleum-based materials. Nevertheless, the extremely high hygroscopicity of cellulose severely degrades their mechanical performance, which is a major obstacle to the production of high-strength, multi-functional cellulose-based materials. In this work, a simple strategy was proposed to fabricate durable versatile nanocellulose films based on sustaining CO2 capture and in-situ calcification. In this strategy, Ca(OH)2 was in-situ formed on the films by Ca2+ crosslinking and subsequent introduction of OH−, which endowed the films with high mechanical strength and carbon sequestration ability. The following CO2 absorption process continuously improved the water resistance and durability of the films, and enabled them to maintain excellent mechanical properties and promising light management ability. After a 30-day CO2 absorption process, the water contact angle of the films can be increased from 43° to 79°, and the weight gain rate of the films in a 30 h water-absorption process can be sharply decreased from 331.2 % to 52.2 %. The films could maintain a high tensile strength of 340 MPa, and result in a CO2 absorption rate of 3.5 mmol/gcellulose after 30 days. In this study, the improvement of durability and carbon sequestration of nanocellulose films was achieved by a simple and effective method. Display omitted