摘要： As the centralized control system of the body, the brain is a complex organ of the utmost importance that even the most minor disorder and trauma can cause inestimable harm. There has always been an unmet clinical need for non-invasive high-resolution imaging techniques without a craniotomy to assist neurosurgeons gain anatomical and functional information for brain examination. Compared to the traditional methods, near-infrared (NIR) imaging (window I, 700–900 nm; window II, 1000–1700 nm) provides an innovative strategy for non-radioactive inspection with high tempo-spatial resolution. In particular, NIR-II imaging shows longer tissue penetration depths and ultralow tissue backgrounds due to drastically decreased photon scattering and tissue autofluorescence. In the current review, we highlight recent advances in NIR fluorophores, especially their rational design and application in NIR fluorescence imaging of the brain, sorted through brain tumors, traumatic brain injuries and bleeding diseases, as well as neurodegenerative disorders like Alzheimer’s and Huntington’s diseases. This state-of-the-art, non-invasive and non-radioactive optical imaging modality shows a promising prospect in understanding the fundamental pathophysiology of neurological diseases and is envisioned for potential clinical translation.