Methods and systems for synthesizing multicompartment capsules are disclosed, as well as multicompartment polymer capsules formed in accordance with disclosed techniques. At least one plurality of polymer capsules are formed via a capsule-forming process. A feed solution and a reservoir solution are provided, each comprising a biopolymer. The feed solution biopolymer and the reservoir solution biopolymer have opposite charges. Droplets of the feed solution are introduced into the reservoir solution, thereby forming via electrostatic complexation a plurality of polymer capsules. At least a portion of the resulting polymer capsules are then encapsulated in a larger polymer capsule via a similar process, wherein the feed solution utilized for the encapsulation process also comprises the formed smaller capsules.