Edible polyelectrolyte microcapsules are constructed from food-grade materials classified as “Generally Recognized as Safe” (GRAS). ε-polylysine (EPL) and polyglutamic acid (PGA) are deposited onto water-soluble sugar–cargo mixtures by an organic solvent-based assembly technique and crosslinked. Cargo-loaded edible microcapsules are created by adding water to dissolve the sacrificial sugar template.