This study reports a significant infrared bulk photovoltaic effect (BPVE) in tellurene (Te) for broad-spectrum neuromodulation. The BPVE in Te spans a wide wavelength range from ultraviolet (390 nm) to mid-infrared (3.8 μm), outperforming previous semiconductors and semimetals in terms of photocurrent density under infrared light simulation (70.4 A cm⁻²). Te nanoflakes successfully elicit action potentials in cortical neurons under broadband light irradiation, demonstrating the potential of Te as a versatile platform for optoelectronic applications and neurological treatments. The mechanism involves the generation of photogenerated electrons and holes, leading to a change in the transmembrane voltage and subsequent neuronal depolarization. This work lays the foundation for further development of infrared BPVE in narrow bandgap materials.This study reports a significant infrared bulk photovoltaic effect (BPVE) in tellurene (Te) for broad-spectrum neuromodulation. The BPVE in Te spans a wide wavelength range from ultraviolet (390 nm) to mid-infrared (3.8 μm), outperforming previous semiconductors and semimetals in terms of photocurrent density under infrared light simulation (70.4 A cm⁻²). Te nanoflakes successfully elicit action potentials in cortical neurons under broadband light irradiation, demonstrating the potential of Te as a versatile platform for optoelectronic applications and neurological treatments. The mechanism involves the generation of photogenerated electrons and holes, leading to a change in the transmembrane voltage and subsequent neuronal depolarization. This work lays the foundation for further development of infrared BPVE in narrow bandgap materials.