The rapidly advancing technology of wearable and miniaturized electronics has increased the demand for low-cost high-performance flexible sensors. Herein, the preparation of translucent freestanding films consisting of cellulose nanofibers (CNFs) and ZnO nanoparticles (NPs) via a simple spray coating method is presented. The obtained nanocomposite films were thin (~10 µm) and flexible. The scanning electron microscopy and atomic force microscopy analysis revealed that the nanocomposite film was composed of regions of ZnO NP-modified CNFs and regions of aggregation of ZnO NPs with each other. The electrical conductance of the films was rapidly increased beyond 40 wt.% ZnO and reached up to >50 nA at 60 wt.% ZnO. This was attributed to the increased number of conductive paths formed by the ZnO NPs in the nanocomposite film when a certain threshold was crossed. The ZnO–CNF nanocomposite film exhibited a stable response over on/off cycles of UV light exposure. The responsivity and sensitivity of the nanocomposite film with 60 wt.% ZnO were 36.5 mA/W and 247, respectively. Even when the device was curved (radius of curvature: 3 mm), the response and sensitivity remained high. The developed nanocomposite films are expected to be applied as environmentally friendly flexible UV sensors.