AbstractThe photovoltaic effect lies at the heart of eco-friendly energy harvesting. However, the conversion efficiency of traditional photovoltaic effect utilizing the built-in electric effect in p-n junctions is restricted by the Shockley-Queisser limit. Alternatively, intrinsic/bulk photovoltaic effect (IPVE/BPVE), a second-order nonlinear optoelectronic effect arising from the broken inversion symmetry of crystalline structure, can overcome this theoretical limit. Here, we uncover giant and robust IPVE in one-dimensional (1D) van der Waals (vdW) grain boundaries (GBs) in a layered semiconductor, ReS₂. The IPVE-induced photocurrent densities in vdW GBs are among the highest reported values compared with all kinds of material platforms. Furthermore, the IPVE-induced photocurrent is gate-tunable with a polarization-independent component along the GBs, which is preferred for energy harvesting. The observed IPVE in vdW GBs demonstrates a promising mechanism for emerging optoelectronics applications.