Developing a cutting-edge system capable of ensuring long-lasting functionality of therapeutic agents and implementing diverse delivery modes is challenging. A quasi-spherical triple-layered capsule containing suspended liquid droplets and allowing multi-modal delivery of therapeutic agents in the aqueous phase was developed, primarily by adopting the core principles for creating liquid marbles. A naturally derived wettable polysaccharide—pectin—was utilized as a liquid–air interfacial barrier to keep the liquid droplets in the core zone. To tailor the pectin-coated droplet as a therapeutic agent carrier, anionic alginate and cationic chitosan layers were sequentially formed via additional interactions: physically stacking substances with structural chirality (pectin–alginate) and inducing electrostatic association to create the reversible complex coacervates (alginate–chitosan). The resulting system, which is called a Chitosan–Alginate–Pectin-coated Suspended-Liquid-Encapsulating (CAPSuLE) marble, had sufficient mechanical strength to resist external harsh environments and exhibited unique features: ecofriendly sustainability, responsiveness to external stimuli, coacervate-driven coalescence for linking adjacent marbles, and a self-repairing ability. The proposed CAPSuLE system can facilitate the adoption of the liquid-marble concept to biomedical fields, extending its applicability in the fields of biology and applied engineering.