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Abstract There is currently enormous and growing demand for flexible electronics for personalized mobile equipment, human–machine interface units, wearable medical‐healthcare systems, and bionic intelligent robots. Cellulose is a well‐known natural biopolymer that has multiple advantages including low cost, renewability, easy processability, and biodegradability, as well as appealing mechanical performance, dielectricity, piezoelectricity, and convertibility. Because of its multiple merits, cellulose is frequently used as a substrate, binder, dielectric layer, gel electrolyte, and derived carbon material for flexible electronic devices. Leveraging the advantages of cellulose to design advanced functional materials will have a significant impact on portable intelligent electronics. Herein, the unique molecular structure and nanostructures (nanocrystals, nanofibers, nanosheets, etc.) of cellulose are briefly introduced, the structure–property–application relationships of cellulosic materials summarized, and the processing technologies for fabricating cellulose‐based flexible electronics considered. The focus then turns to the recent advances of cellulose‐based functional materials toward emerging intelligent electronic devices including flexible sensors, optoelectronic devices, field‐effect transistors, nanogenerators, electrochemical energy storage devices, biomimetic electronic skins, and biological detection devices. Finally, an outlook of the potential challenges and future prospects for developing cellulose‐based wearable devices and bioelectronic systems is presented.