Understanding the detailed functioning and pathophysiology of the brain and the nervous system continues to challenge the scientific community, particularly in terms of scaling up techniques for monitoring and interfacing with complex 3D networks. Nanotechnology has the potential to support this scaling up, where the eventual goal would be to address individual nerve cells within functional units of both the central and peripheral nervous system. Gold nanoparticles provide a variety of physical and chemical properties that have attracted attention as a light-activated nanoscale neuronal interface. This review provides a critical overview of the photothermal and photomechanical properties of chemically functionalized gold nanoparticles that have been exploited to trigger a range of biological responses in neuronal tissues, including modulation of electrical activity and nerve regeneration. The prospects and challenges for further development are also discussed.