In this paper, (1) a simple and controllable method to synthesize single crystalline nanoribbons of CuTCNQ in a large area was demonstrated by using a physical and chemical vapor combined deposition technique. (2) Nanoribbons synthesized by this method were identified to belong to phase I. (3) Devices and device arrays of nanoribbons were in situ fabricated by this method using gap electrodes and gap electrode arrays. (4) Current-voltage characteristics of crystalline devices and device arrays of nanoribbons exhibited semiconductor properties, and this conclusion was further confirmed by the results of devices based on an individual nanoribbon or microribbon of CuTCNQ (phase I). The controllable synthesis of nanoribbons for the in situ fabrication of crystalline nanodevices and device arrays will be attractive for nanoelectronics. Moreover, semiconductor current-voltage characteristics of the nanoribbons will be beneficial to the understanding of CuTCNQ.