Multilayer MoS 2 is a promising active material for sensing, energy harvesting, and optoelectronic devices owing to its intriguing tunable electronic band structure. However, its optoelectronic applications have been limited due to its indirect band gap nature. In this study, we fabricated a new type of phototransistor using multilayer MoS 2 crystal hybridized with p-type organic semiconducting rubrene patches. Owing to the outstanding photophysical properties of rubrene, the device characteristics such as charge mobility and photoresponsivity were considerably enhanced to an extent depending on the thickness of the rubrene patches. The enhanced photoresponsive conductance was analyzed in terms of the charge transfer doping effect, validated by the results of the nanoscale laser confocal microscope photoluminescence (PL) and time-resolved PL measurements.