Optoelectronic neuromodulation has transformed neuroscience research and holds great promise for treating neurological disorders. However, conventional optoelectronic methods rely on ultraviolet/visible light, which poorly penetrates tissue and typically necessitates surgically implanted optical fibers for deep-brain stimulation. Here, a heterostructure is presented that integrates near-infrared (NIR)-excitable upconversion nanoparticles (UCNPs) and broadband-absorbing CsPbBr3 perovskite quantum dots (QDs). This nanostructure converts deeply penetrating 980 nm NIR light into localized electrical stimuli, enabling immediate and precise modulation of neuronal activity without implants. In vitro, NIR illumination of this heterostructure reliably increases the firing rate of wild-type dopaminergic (DA) neurons in acute brain slices. Importantly, in vivo, transcranial NIR stimulation of the heterostructure in the secondary motor cortex (M2) and ventral tegmental area (VTA) modulates neuronal activity, triggers turning behavior, and promotes dopamine release. Moreover, it exhibits negligible neuroinflammation and structural stability in brain tissue over at least four weeks. By integrating a stable heterostructure for efficient NIR-driven photocurrent generation, the method offers a non-genetic, minimally invasive platform for precise neuromodulation in wild-type animals.