Gold nanoparticle (Au-NP)-based colorimetric assays offer new opportunitites for the visualization and quantification of neurochemicals involved in physiological and pathological processes due to their high sensitivity, designability, and low technical demands. In this Research News, we systematically review the advances on the development of Au-NP-based colorimetric methods for visualization and quantification of neurochemicals and their potential applications for effectively monitoring neurochemicals in the central nervous system. By integration of the favourable surface chemistry with the high extinction coefficient of Au-NPs, some new principles and methods could be developed for the quantification of neurochemicals involved in brain functions. New strategies to design the surface chemistry of Au-NPs, along with the key challenges yet to be addressed to achieve online visualization and quantification of neurochemicals in the central nervous system, are illustrated and discussed. The questions opened here should inspire future investigations and lead to discoveries that continue the development of the effective analytical protocols based on Au-NPs for neurochemical visualization and quantification.