Cellulose and its derivatives have evoked much attention in sensor technology as host-matrices for conducting materials because of their versatility, renewability, and biocompatibility. However, only a few studies have dealt with the potential utilization of cellulose as a sensing material without a composite structure. In this study, cellulose nanofibers (CNF) and 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO)-oxidized cellulose nanofibers (TOCNF) extracted from rice husks by using ultrasonic-assisted methods are introduced as a potential gas sensing material with highly sensitive performance. To fabricate nanocellulose-based films, CNF, TOCNF, and TOCNF with glycerol (TOCNF/G) were dispersed in water and applied on polyimide substrate with digital electrodes to form self-standing thin films by a drop-casting method. A transparent coating layer on the surface of the plate after drying is used for the detection of water-soluble gases such as acetone, ammonia, methane, and hydrogen sulfide gases at room temperature at 52% relative humidity. The sensor prototypes exhibited high sensitivity, and the detection limit was between 1 ppm and 5 ppm, with less than 10 min response and recovery time. The results indicate that both the CNF- and the TOCNF-coated sensors show good sensitivity toward ammonia and acetone, compared to other gases. A TOCNF/G-coated sensor exhibited minimum time in regard to response/recovery time, compared to a CNF-coated sensor. In this study, nanocellulose-based sensors were successfully fabricated using a low-cost process and a bio-based platform. They showed good sensitivity for the detection of various gases under ambient conditions. Therefore, our study results should further propel in-depth research regarding various applications of cellulose-based sensors in the future.