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Substantial progress in flexible or stretchable electronics over the past decade has extensively impacted various technologies such as wearable devices, displays and automotive electronics for smart cars. An important challenge is the reliability of these deformable devices under thermal stress. Different coefficients of thermal expansion (CTE) between plastic substrates and the device components, which include multiple inorganic layers of metals or ceramics, induce thermal stress in the devices during fabrication processes or long-term operations with repetitions of thermal cyclic loading–unloading, leading to device failure and reliability degradation. Here, we report an unconventional approach to form photo-patternable, transparent cellulose nanofiber (CNF) hybrid films as flexible and stretchable substrates to improve device reliability using simultaneous electrospinning and spraying. The electrospun polymeric backbones and sprayed CNF fillers enable the resulting hybrid structure to be photolithographically patternable as a negative photoresist and thermally and mechanically stable, presenting outstanding optical transparency and low CTE. We also formed stretchable origami substrates using the CNF hybrid that are composed of rigid support fixtures and elastomeric joints, exploiting the photo-patternability. A demonstration of transparent organic light-emitting diodes and touchscreen panels on the hybrid film suggests its potential for use in next-generation electronics.