This article presents an overview of the current progress in molecular mimetic self-assembly of colloidal particles. Firstly, the recent study of colloidal particles at interfaces is highlighted, underlining the mesoscopic mimicry of the surface activity of amphiphilic molecules using colloidal particles. Secondly, various strategies developed thus far to impart colloidal particles with anisotropy in terms of chemical composition, surface chemistry and particle morphology, which are regarded as mesoscopic atoms and molecules, are reviewed. Thirdly, an overview of the current theoretical and experimental results of using the rules of molecular synthesis and self-assembly to direct self-assembly of colloidal particles is presented. Finally, the experimental challenges associated with molecular mimetic self-assembly of colloidal particles are outlined, giving a rather conservative conclusion of the status quo of this new research field with a very optimistic outlook.