AbstractThe study of organic semiconductor single crystal (OSSC) arrays has recently attracted considerable interest given their potential applications in flexible displays, smart wearable devices, biochemical sensors, etc. Patterning of OSSCs is the prerequisite for the realization of organic integrated circuits. Patterned OSSCs can not only decrease the crosstalk between adjacent organic field‐effect transistors (OFETs), but also can be conveniently integrated with other device elements which facilitate circuits application. Tremendous efforts have been devoted in the controllable preparation of OSSC arrays, and great progress has been achieved. In this review, the general strategies for patterning OSSCs are summarized, along with the discussion of the advantages and limitations of different patterning methods. Given the identical thickness of monolayer molecular crystals (MMCs) which is beneficial to achieve super uniformity of OSSC arrays and devices, patterning of MMCs is also emphasized. Then, OFET performance is summarized with comparison of the mobility and coefficient of variation based on the OSSC arrays prepared by different methods. Furthermore, advances of OSSC array‐based circuits and flexible devices of different functions are highlighted. Finally, the challenges that need to be tackled in the future are presented.