This study reports a giant infrared bulk photovoltaic effect (BPVE) in tellurine (Te) for broad-spectrum neuromodulation. Te, a narrow bandgap semiconductor, exhibits a wide range of photovoltaic wavelengths from ultraviolet to mid-infrared, with a photocurrent density of 70.4 A cm⁻² under infrared light, surpassing previous semiconductors and semimetals. The BPVE in Te is attributed to its noncentrosymmetric structure, which enables efficient light-to-electricity conversion. Te nanoflakes, when attached to cortical neurons, elicit action potentials under broad-spectrum light irradiation, demonstrating the potential of Te for neuromodulation. The study also reveals that the BPVE in Te spans a wide wavelength range, from ultraviolet (390 nm) to mid-infrared (3.8 μm), and that the infrared BPVE in Te is highly efficient, enabling broad-spectrum neuromodulation. The results suggest that Te could be a promising candidate for optoelectronic applications and neuromodulation therapies. The study highlights the potential of Te for infrared-based optoelectronic applications and neuromodulation, with the BPVE in Te providing a versatile platform for exploring optoelectronic applications. The findings demonstrate that Te can be used for broad-spectrum neuromodulation, with the BPVE in Te enabling efficient light-to-electricity conversion and neuromodulation. The study also shows that Te can be used for neuromodulation, with the BPVE in Te enabling efficient light-to-electricity conversion and neuromodulation. The results suggest that Te could be a promising candidate for optoelectronic applications and neuromodulation therapies.This study reports a giant infrared bulk photovoltaic effect (BPVE) in tellurine (Te) for broad-spectrum neuromodulation. Te, a narrow bandgap semiconductor, exhibits a wide range of photovoltaic wavelengths from ultraviolet to mid-infrared, with a photocurrent density of 70.4 A cm⁻² under infrared light, surpassing previous semiconductors and semimetals. The BPVE in Te is attributed to its noncentrosymmetric structure, which enables efficient light-to-electricity conversion. Te nanoflakes, when attached to cortical neurons, elicit action potentials under broad-spectrum light irradiation, demonstrating the potential of Te for neuromodulation. The study also reveals that the BPVE in Te spans a wide wavelength range, from ultraviolet (390 nm) to mid-infrared (3.8 μm), and that the infrared BPVE in Te is highly efficient, enabling broad-spectrum neuromodulation. The results suggest that Te could be a promising candidate for optoelectronic applications and neuromodulation therapies. The study highlights the potential of Te for infrared-based optoelectronic applications and neuromodulation, with the BPVE in Te providing a versatile platform for exploring optoelectronic applications. The findings demonstrate that Te can be used for broad-spectrum neuromodulation, with the BPVE in Te enabling efficient light-to-electricity conversion and neuromodulation. The study also shows that Te can be used for neuromodulation, with the BPVE in Te enabling efficient light-to-electricity conversion and neuromodulation. The results suggest that Te could be a promising candidate for optoelectronic applications and neuromodulation therapies.