Importantly, the ultralow thickness of a 2D organic semiconductor is essential for high-performance phototransistors as it warrants higher charge carrier mobility and faster photoresponse time based on the efficient charge injection and short interlayer recombination distance for trapped charge carriers, respectively. [10,13] In order to develop color-filter-free photodetectors and image sensors, wavelength-selective organic semiconductors in red, green, and blue have been widely investigated, but none of them are based on the crystalline 2D organic semiconductors. [14][15][16][17][18][19] In other words, to the best of our knowledge, 2D organic phototransistors showing green-sensitive absorption for hybrid CMOS image sensor application are yet to be developed. Recently, however, some nonvisible wavelength-selective organic 2D phototransistors have been reported, which respond to either ultraviolet (UV) or near-infrared (NIR) irradiation. Liu et al. reported hybrid phototransistors by growing a few mono layers of dioctylbenzothienobenzothiophene (C8-BTBT) as a UV absorbing layer on a charge-transporting graphene layer by the chemical vapor deposition method. [10] Due to the high charge carrier mobility of graphene and efficient charge separation property of the monolayer of C8-BTBT, they achieved responsivity of 1.57 × 10 4 A W −1 and ultrafast response time of 25 ms under 355 nm laser irradiation. Cao et al. also reported UV absorbing 2D organic phototransistors based on 1,4-bis(4methylstyryl)benzene (p-MSB) by a drop casting method. [12] They found that the internal photoresponsivity of the 2D phototransistors was as high as 2.13 × 10 5 A W −1 under 365 nm light irradiation, which was about two to three orders higher than that of bulk crystals. Wang et al. prepared a few monolayers thick NIR absorbing furan-thiophene quinoidal compound (TFT-CN) by the solution epitaxy method. [11] After transferring the TFT-CN 2D crystal from the water surface to the SiO 2 /Si wafer, they successfully demonstrated high-performing NIR phototransistors with responsivity of up to 9 × 10 4 A W −1 and very low dark current of 0.3 pA under 808 nm laser irradiation. Such high-performance demonstrations in UV and NIR organic 2D phototransistors strongly suggest that 2D phototransistors could be an excellent platform for the full-color CMOS image sensors, specifically for the green-selective 2D organic phototransistors for stacked CMOS architectures. Recently, scientific interests in 2D organic semiconductors have been rapidly growing, and a few review papers are already available. [20,21] In order to establish a design strategy for green-sensitive 2D materials, we examined the structure-property relationship 2D single crystals of down to two-monolayer thickness are fabricated from a push-pull structure-based green light absorbing organic n-type semiconductor, (2E,2′E)-3,3′-(2,5-difluoro-1,4-phenylene)bis(2-(5-(4-(trifluoromethyl) phenyl)thiophen-2-yl)acrylonitrile) (2F-4-TFPTA). The 2F-4-TFPTA 2D single crystal exhibits field-effect el...