Flexible thin-film organic semiconductor devices have received wide attention due to favorable properties such as light-weight, flexibility, reproducible semiconductor resources, easy tuning of functional properties via molecular tailoring, and low cost large-area solution-procession. Among them, ultraflexible electronics, usually with minimum bending radius of less than 1 mm, are essential for the development of epidermal and bio-implanted electronics, wearable electronics, collapsible and portable electronics, three dimensional (3D) surface compliable electronics, and bionics. This review firstly gives a brief introduction of development from flexible to ultraflexible organic semiconductor electronics, and design of ultraflexible devices, then summarizes the recent advances in ultraflexible thin-film organic semiconductor devices, focusing on organic field effect transistors, organic light-emitting diodes, organic solar cells and organic memory devices.