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Absorbing near‐infrared (NIR) photons, with longer wavelengths, in atomically thin monolayer MoS2 presents a significant challenge due to its weak optical absorption and narrow absorption bands. Consequently, MoS2‐based photodetector devices often experience low responsivity and a limited detection window. Herein, a novel InAs@ZnSe core@shell/1L‐MoS2 heterostructure, leveraging InAs@ZnSe as the primary infrared‐absorbing material and exploiting the formation of a type‐II heterostructure is showcased. Steady‐state and time‐resolved spectroscopy, along with optoelectronic characterization, are employed to investigate photo‐induced charge transfer dynamics. The results show efficient hole transfer to InAs@ZnSe upon excitation of both materials. Instead, with selective excitation of InAs@ZnSe, electron transfer is observed from InAs@ZnSe to the 1L‐MoS2. The heterostructure demonstrates a broadband photoresponse spanning the wavelength range of 300 to 850 nm, exhibiting a Responsivity of ≈103 A/W and Detectivity of ≈1011 Jones. The signal‐to‐noise ratio substantially increases by 3 to 4 orders of magnitude for 700 and 850 nm excitation compared to pristine 1L‐MoS2. The enhancement in photoresponse and signal‐to‐noise ratio is attributed to increased absorption, which helps eliminate defect and trap states, thereby promoting the photogating effect. [ABSTRACT FROM AUTHOR]