Two-dimensional
(2D) photodetectors based on photovoltaic effect
or photogating effect can hardly achieve both high photoresponsivity
and large linear dynamic range at the same time, which greatly limits
many practical applications such as imaging sensors. Here, the conductive-sensitizer
strategy, a general design for improving photoresponsivity and linear
dynamic range in 2D photodetectors is provided and experimentally
demonstrated on vertically stacked bilayer WS2/GaS0.87 under a parallel circuit mode. Owing to successful band
alignment engineering, the isotype type-II heterojunction enables
efficient charge carrier transfer from WS2, the high-mobility
sensitizer, to GaS0.87, the low-mobility channel, under
illumination from a broad visible spectrum. The transferred electron
charges introduce a reverse electric field which efficiently lowers
the band offset between the two materials, facilitating a transition
from low-mobility photocarrier transport to high-mobility photocarrier
transport with increasing illumination power. We achieved a large
linear dynamic range of 73 dB as well as a high and constant photoresponsivity
of 13 A/W under green light. X-ray photoelectron spectroscopy, cathodoluminescence,
and Kelvin probe force microscopy further identify the key role of
defects in monolayer GaS0.87 in engineering the band alignment
with monolayer WS2. This work proposes a design route based
on band and interface modulation for improving performance of 2D photodetectors
and provides deep insights into the important role of strong interlayer
coupling in offering heterostructures with desired properties and
functions.