Eco‐friendly and low‐cost cellulose nanofiber paper (nanopaper) is a promising candidate as a novel substrate for flexible electron device applications. Here, a thin transparent nanopaper‐based high‐mobility organic thin‐film transistor (OTFT) array is demonstrated for the first time. Nanopaper made from only native wood cellulose nanofibers has excellent thermal stability (>180 °C) and chemical durability, and a low coefficient of thermal expansion (CTE: 5–10 ppm K ‐1 ). These features make it possible to build an OTFT array on nanopaper using a similar process to that for an array on conventional glass. A short‐channel bottom‐contact OTFT is successfully fabricated on the nanopaper by a lithographic and solution‐based process. Owing to the smoothness of the cast‐coated nanopaper surface, a solution processed organic semiconductor film on the nanopaper comprises large crystalline domains with a size of approximately 50–100 μm, and the corresponding TFT exhibits a high hole mobility of up to 1 cm 2 V ‐1 s ‐1 and a small hysteresis of below 0.1 V under ambient conditions. The nanopaper‐based OTFT also had excellent flexibility and can be formed into an arbitrary shape. These combined technologies of low‐cost and eco‐friendly paper substrates and solution‐based organic TFTs are promising for use in future flexible electronics application such as flexible displays and sensors.