Iodide ions have been used as an additive to fabricate homogeneous gold spheres with a la carte dimensions, ranging from the nano- (50 nm) to the microscale (ca. 1 mu m). Due to the high uniformity and surface functionalization of the produced materials, they undergo spontaneous assembly into organized superlattices upon solvent drying. Thus, optical properties of the particles including localized surface plasmon resonances and surface enhanced Raman scattering (SERS) response, both in solution and organized into superlattices, are also reported.