Organic electronics with π-conjugated organic semiconductors are promising candidates for the next electronics revolution. For the conductive channel, the large-area two-dimensional (2D) crystals of organic semiconductors (2DCOS) serve as useful scaffolds for modern organic electronics, benefiting not only from long-range order and low defect density nature but also from unique charge transport characteristic and photoelectrical properties. Meanwhile, the solution process with advantages of cost-effectiveness and room temperature compatibility is the foundation of high-throughput print electrical devices. Herein, we will give an insightful overview to witness the huge advances in 2DCOS over the past decade. First, the typical influencing factors and state-of-the-art assembly strategies of the solution-process for large-area 2DCOS over sub-millimeter even to wafer size are discussed accompanying rational evaluation. Then, the charge transport characteristics and contact resistance of 2DCOS-based transistors are explored. Following this, beyond single transistors, the p-n junction devices and planar integrated circuits based on 2DCOS are also emphasized. Furthermore, the burgeoning phototransistors (OPTs) based on crystals in the 2D limits are elaborated. Next, we emphasized the unique and enhanced photoelectrical properties based on a hybrid system with other 2D van der Waals solids. Finally, frontier insights and opportunities are proposed, promoting further research in this field.
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