been shown to be promising in other different applications, including organic logic circuits, memory devices, various sensors, medical applications, and display drivers. [1][2][3][4][6][7][8][9][10][11] Solution processing approaches for the growth of high-quality organic thin films of up to a wafer-scale size have been reported by several groups. [3,12] However, to fully utilize the advantages of highly crystalline organic semiconductors, large-area deposition is not enough; availability of ultrathin films, or even films with the thickness of down to a single molecular layer, is also very important for reducing the access contact resistance. This is necessary for maintaining the high-speed operation (especially in the staggered top-contact/bottom-gate OFETs), while further shrinking the device size dictated by the overall circuit miniaturization. Recently, we have successfully demonstrated a sub-thermionic subthreshold swing and a high-current-density operation of OFETs based on monolayers of a p-type organic semiconductor, 2,9-didecyldinaphtho[2,3-b:2',3'-f]thieno [3,2-b]thiophene (C 10 -DNTT), used as the active layer. [13,14] In addition, the impactful studies on the monolayer molecular crystals (MMCs) have been conducted broadly. The excellent optical properties of MMCs enable the highperformance optoelectronics. [15,16] Sensitive to the external stimuli owing to the ultrathin feature, the MMCs provide promising candidate for sensor application. [9,17] Meanwhile, the ultrathin smooth surfaces of MMCs allow the high-quality p-n junction and logic circuits. [18,19] In this communication, we investigate the origin of the low contact resistance observed