J-aggregates are fantastic self-assembled chromophores with a very narrow and extremely sharp absorbance band in the visible and near-infrared spectrum, and hence they have found many exciting applications in nonlinear optics, sensing, optical devices, photography, and lasing. In silver halide photography, for example, they have enormously improved the spectral sensitivity of photographic process due to their fast and coherent energy migration ability. On the other hand, graphene, consisting of single layer of carbon atoms forming a hexagonal lattice, has a very low absorption coefficient. Inspired by the fact that J-aggregates have carried the role to sense the incident light in silver halide photography, we would like to use Jaggregates to increase spectral sensitivity of graphene in the visible spectrum. Nevertheless, it has been an outstanding challenge to place isolated J-aggregate films on graphene to extensively study interaction between them. We herein noncovalently fabricate isolated J-aggregate thin films on graphene by using a thin film fabrication technique we termed here membrane casting (MC). MC significantly simplifies thin film formation of water-soluble substances on any surface via porous polymer membrane. Therefore, we reversibly modulate the Dirac point of graphene in the J-aggregate/graphene van der Waals (vdW) heterostructure and demonstrate an all-carbon phototransistor gated by visible light. Owing to the hole transfer from excited excitonic thin film to graphene layer, graphene is hole-doped. In addition, spectral and power responses of the all-carbon phototransistor have been measured by using a tunable laser in the visible spectrum. The first integration of J-aggregates with graphene in a transistor structure enables one to reversibly write and erase charge doping in graphene with visible light that paves the way for using J-aggregate/graphene vdW heterostructures in optoelectronic applications.