Nanoporous membranes are used as templates for polyelectrolyte encapsulation of colloidal nanoparticles, leading to colloidally dispersible, multifunctional, and multicompartment microfibers. The protocol is simple and independent of the chemical nature of the nanoparticles and polyelectrolytes. Furthermore, the surface polyelectrolyte coating allows free transfer of the resulting microfibers into various aqueous and organic media.