near-infrared (NIR) optical region and beyond. Then, in order to broaden the response spectrum range and improve the photoresponse of MoS 2 , van der Waals (vdWs) heterostructure-composed MoS 2 with another TMDC have been extensively and deeply investigated to make full use of not only the enhanced light absorption but also the interlayer interaction between the composed layers under light. [9][10][11][12][13] Lateral vertically stacked WS 2 /MoS 2 hybrid photodetectors with graphene as contact have achieved a photoresponsivity and photoconductive gain as high as 10 3 A W −1 and 3 × 10 4 , respectively. [14] The proposed WSe 2 /MoS 2 phototransistor has exhibited an excellent performance with specific detectivity of 5 × 10 11 Jones, high photoresponsivity of 2.7 × 10 3 A W −1 , and response time of 0.017 s. [15] Jung and co-workers reported an enhanced dye-sensitized solar cell with 8.07% conversion efficiency attained for MoS 2 /MoTe 2 counter electrode. [16] Besides those, multilayer ReSe 2 /MoS 2 p-n photodetectors showed a high photoresponsivity of 6.75 A W −1 and external quantum efficiency over 1200%. [17] It is also important to emphasize that these heterojunctions can make the photogenerated carriers separation more efficient by the aid of builtin electric field at the interface, which in turn improved the photodetection performance.Besides group-VI TMDCs, group-X TMDCs mainly including PtS 2 /Se 2 and PdS 2 /Se 2 have recently come under the spotlight as representative of stable TMDCs and attracted an increasing attention due to their superior properties, for example, wide spectrum range, good air stability, high carrier mobility, and strong interlayer interaction, and so on. [18][19][20][21][22] Group-X TMDCs are predicted to be promising semiconductors with narrow bandgap 0-0.25 eV in bulk and room-temperature carrier mobility higher than 1000 cm 2 V −1 s −1 by theoretical calculation. [23][24][25] Among them, PdSe 2 has emerged as a new 2D material for broadband spectrum photodetection with a strong thickness-dependent bandgap of 0-1.4 eV from bulk to monolayer. Specifically, it also possesses a pentagonal puckered structure which endows it strong in-plane anisotropic mechanical, optical, electrical, and thermal properties. [21,26] For photodetection, the PdSe 2 NIR photodetector shows a photoresponsivity of 660 A W −1 under 914 nm laser and the electrical property after 6 months keeping in the air show little change as published by Recently, group-X transition metal dichalcogenides with tunable distinct optical and superior electrical properties have displayed profound potential in various optoelectronic devices. In this work, novel van der Waals (vdWs) heterostructures composed of monolayer MoS 2 and few-layer PdSe 2 grown by chemical vapor deposition are employed in photodetectors for broadband and polarized photodetection. Excitingly, optoelectronic measurements show that the MoS 2 /PdSe 2 photodetector is sensitive to near-infrared light with responsivity as high as 6.9 A W −1 , specific detectiv...