||Charge-transfer (CT) complexes have been studied for several decades as a result of the unique chemical and physical properties. And organic CT complexes have demonstrated their ability to serve as OFET materials, with tunable Fermi energies. More in-depth study of this concept and its application in conjunction with other organic semiconductors may provide a solution for one of the most difficult bottlenecks in organic device research for establishing efficient charge mobility. Further progress is necessary in several areas. First, an improved crystallinity of CT complex is available relating the structure of CT complexes to their electronic properties. At the same time, development of less-complex processing methods for such materials is desired in order for them to be able to sustain low-cost fabrication of organic devices. Herein, we report an approach to fabricate organic CT complexes of highly crystallinity by eutectic crystallization.