We have devised in this work a general synthetic strategy for preparation of single- and multicomponent rare-earth coordination.. polymer colloidal spheres (RE-CPCSs). This strategy is based on an integration of coordination chemistry and antisolvent effect for synchronized precipitation. Highly monodisperse RE-CPCSs with homogeneous mixing of RE elements, which are not readily attainable by any existing methods, have been successfully prepared for the first time. In addition, the type and molar ratio of these colloidal spheres can be adjusted easily in accordance to the variety and dosage of precursor salts. The molar ratio of RE elements in as-prepared colloidal spheres shows a linear relationship to that of starting reactants. Furthermore, the RE-based core/shell colloidal spheres can be facilely prepared by introducing other metal salts (beyond lanthanide elements) owing to their different coordination chemistry and precipitation behavior. By adjusting concentrations of the ionic activators, luminescent properties can be tuned accordingly. Moreover, the RE-CPCSs can be transformed to monodisperse lanthanide oxide spheres via simple heat treatment. We believe that the present synthetic strategy provides a viable route to prepare other lanthanide-containing colloidal spheres that have enormous potential for future applications as optoelectronic devices, catalysts, gas sensors, and solar cells.