The bottom-up fabrication of facile, lower-cost, larger areas optical metamaterials (OMMs) is expected to provide important benefits for applications in stealth technology and communication networks. Currently available OMMs at optical wavelengths are all composed of periodic structures, and fabricated by top-down approaches of e-beam lithography or focused ion beam technique. Limited by the high cost and extremely small sample volumes size, the fabrication of visible OMMs is still quite challenging on the nanometer scale. The rapid maturation of synthetic methodology in the field of the nanometer scale has lead to the creation of new materials at an incredible rate. In this review, we regard a V-shaped core as an artificial atom and a dendritic cell as an artificial molecule, and address the bottom-up fabrication and performance of optical metamaterials, and with an outlook toward developing devices capable of operating in optical media.