Flexible and highly sensitive humidity sensors are crucial for humidity detection. In this study, a flexible cellulose nanofiber/carbon nanotube (NFC/CNT) humidity sensor with high sensitivity performance was developed via fast vacuum filtration. CNTs were well dispersed in water by using 2,2,6,6-tetramethylpiperidinyl-1-oxyl (TEMPO)-oxidized NFC as a dispersant. More importantly, NFC also acted as a humidity sensitive material, achieving superior performance of NFC/CNT humidity sensors. The obtained NFC/CNT humidity sensor with 5 wt % CNT loading exhibits outstanding sensitive performance, and its response value reaches a maximum of 69.9% (Delta I/I-0) at 95% relative humidity (RH). It also displays good bending resistance and long-term stability. In addition, the NFC/CNT humidity sensor was employed to monitor human breath. Therefore, we believe that the flexible, highly sensitive, and simply designed NFC/CNT humidity sensor is a promising candidate for various applications in the field of humidity measurement.