van der Waals heterostructures of two-dimensional (2D) materials have attracted considerable attention due to their flexibility in the design of new functional devices. Despite numerous studies on graphene/2D semiconductor heterostructures, their optoelectronic applications are significantly hindered because of several disadvantages, such as large band gaps and chemical instability. In this work, we demonstrate the fabrication of graphene/S-doped InSe heterostructure photodetectors with excellent photoresponse performance, and this is attributed to the moderate band gap and band gap engineering by element doping of InSe as well as the high carrier mobility of graphene. In particular, the graphene/InSe0.9S0.1 device achieves an ultrahigh photoresponsivity of ∼4.9 × 106 A W-1 at 700 nm and an EQE of 8.7 × 108%, and it exhibits broadband photodetection (visible to near-infrared). More importantly, by virtue of the interaction between n-type graphene arising from the influence of h-BN as a dielectric layer and S-doped InSe with a high work-function, our devices always exhibited positive photocurrent when the polarity of the gate voltage is adjusted, and is different from that the previously reported graphene/2D semiconductor photodetectors. This work not only provides a promising platform for highly efficient broadband photodetectors but also sheds light on tuning the optoelectronic performance through band gap engineering and designing novel heterostructures-based various 2D materials.