Abstract2D van der Waals (vdWs) heterojunctions exhibit facile fabrication process and tunable optoelectronic properties. However, suppressing interfacial charge traps and multifunctional photoresponse remain significant challenges. Here, the study designs a 2D multifunctional phototransistor based on ambipolar MoTe2/graphene (Gr)/p‐type SnS0.25Se0.75 double vdWs vertical heterostructure via alloy engineering. The middle Gr interlayer is pivotal in reducing interfacial charge traps, facilitating vertical photocarrier transportation, and enhancing light absorption coefficient. Under photogating effect, the trapped electrons in SnS0.25Se0.75 promote the photogating effect, resulting in the maximum photogain of 8084 and specific detectivity (D*) of 8.2 × 1012 Jones. Under photoconductive effect, a high responsivity (R) of 36.9 A W−1 and D* of 7.17 × 1011 Jones are achieved. Under photovoltaic effect, the devices exhibit a remarkable R of 501 mA W−1, D* of 1.4 × 1011 Jones. Notably, a self‐driven photocurrent polarized ratio of 8 under 635 nm is achieved because of the anisotropic nature of SnS0.25Se0.75 and the effective double built‐in electric fields. By varying the gate voltage, the polarization ratio can be modulated from 1 to 2.5, enabling reconfigurable polarized‐sensitive detection. Above all, the designed heterojunction with multifunctional and reconfigurable polarization detection.
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