Unidirectional dewetting enables the production of large-area thin films with high efficiency at low cost. Herein, we report homogeneous unidirectional dewetting on large-area microdroplet arrays via gravity-induced deformation in droplets combined with alternating lyophilic/lyophobic patterns. This process allows the scaled-up deposition of thin films, including organic semiconductors and transition metal oxides, through the autogenous shrinkage of droplets, which further enables the fabrication of large-area organic thin-film transistor (OTFT) arrays. The resulting field-effect mobility and on/off ratio of the fully printed OTFTs exceeded 13 cm 2 V − 1 s − 1 and 10 8 , respectively. Therefore, the presented dewetting method is promising to realize the roll-to-roll manufacture of large-area flexible electronics.