Angiogenin (ANG) is a ribonuclease that plays a crucial role in various physiological processes in the brain and the development of neurological diseases. ANG is widely expressed in different brain cells, including neurons, the endothelium of cerebral blood vessels, and glial cells. It exhibits a wide range of mechanisms, such as promoting the formation of new blood vessels, reducing oxidative stress, suppressing inflammation, promoting tissue repair, stimulating cell growth, and inhibiting cell death. These findings suggest that ANG has the potential to be used as a therapeutic agent for neurological diseases. This review aims to explore the physiological functions of ANG in the brain and its pathological roles in neurological disorders, with the ultimate goal of identifying potential future neuroprotection strategies.