The NIR photoresponse of the Gr/MoSe2/Si device was further assessed by using the 808, 1064, and 1310 nm lasers as light sources. In Figure 4e, the device exhibits remarkable photoresponse to 808 and 1064 nm lasers. However, photoresponse becomes weaker for the 1310 nm laser since its energy (0.95 eV) is already smaller than the bandgap of MoSe2 film (1.1 eV). Significantly, owing to the pronounced photovoltaic behavior, the device can operate at zero bias voltage with excellent reproducibility and stability (Figure 4f). The step rise and fall edges to pulsed light also reveal that the photocurrent and photo‐induced voltage are originated from photovoltaic effect, instead of bolometric effect.