Abstract: The invention is directed to (i) the encapsulation of uncharged organic substances in polymeric capsules by using a multi-step strategy that involves charging the surface of the microcrystals with an amphiphilic substance, followed by consecutively depositing polyelectrolytes of opposite charge to assemble a multilayered shell of polymeric material around the microcrystal template, and (ii) the formation of polymer multilayer cages derived from the coated crystals by facile removal of the crystalline template.