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Van der Waals heterostructures composed of transition-metal dichalcogenide (TMD) materials have become a remarkable compact system that could offer an innovative architecture for advanced engineering in high-performance energy-harvesting and optoelectronic devices. Here, we report a novel van der Waals (vdW) TMD heterojunction photodiode composed of black phosphorus (p-BP) and palladium diselenide (n-PdSe2), which establish a high and tunable rectification and photoresponsivity. A high rectification up to ≈7.1 × 105 is achieved, which i