The facile fabrication of thin and foldable self‐healing electronics on a poly(vinyl alcohol)/cellulose nanocrystal (PVA/CNC) composite film is reported. The self‐healing property of the PVA/CNC nanocomposite film can be activated by spraying water on the film surface, via dynamic formation of hydrogen bonding. The self‐healing efficiency of PVA/CNC is influenced by the content of CNC in the film, pH of the spraying solution, and the temperature. Via vacuum filtration and pattern transfer techniques, both a supercapacitor and a temperature sensor are fabricated on the same PVA/CNC film using gold nanosheet (AuNS) and polyaniline/multiwalled nanotube (PANI/MWCNT) electrodes. The fabricated supercapacitor with a gel‐type electrolyte exhibits a high electrochemical performance, and the thermoresistive temperature sensor shows a linear sensitivity with a fast response. Both devices exhibit superior mechanical stability and self‐healing property over 100 repetitive folding and five repetitive healing cycles, respectively, retaining the device performance owing to the percolated network of the conductive materials. This work demonstrates that our paper‐like thin PVA/CNC film‐based self‐healable devices can serve as highly durable and deformable electronics with longevity. A paper‐like, thin, foldable, and self‐healable electronic based on poly(vinyl alcohol)/cellulose nanocrystal (PVA/CNC) nanocomposite film shows a water‐stimulated self‐healing property due to dynamic hydrogen bonding formation. A high‐performance planar supercapacitor and thermoresistive temperature sensor fabricated on the PVA/CNC substrate exhibits a high electrical self‐healing property after complete bisection as well as high mechanical stability under repetitive folding deformation.