Vesicles were generated using a modified continuous droplet interface crossing encapsulation (cDICE) method (Figure , see Supporting Information). In short, it is an emulsion-based method where monolayers in water-in-oil droplets acquire a second monolayer at the oil-water interface through centrifugal force by van der Waals attraction. Poly(ethylene oxide)-b-polybutadiene (PEO14-b-PBD22, MW = 1.8 kDa, hereafter referred to as PEO-PBD) was selected as the block copolymer as it is a well-established amphiphilic polymer for hybrid vesicle formation. 1.8 kDa sized PEO-PBD was used, as its similar thickness to lipid membrane helps minimize the mismatch between lipid and polymer. PEO-PBD was mixed with 1,2-dioleoyl-sn-glycero-3-phophocholine (DOPC) at 50/50 mol% to produce phospholipid-block copolymer hybrid vesicles. Generated vesicles had an average size of ~21.0 ± 8.5 μm (Figure ), and had significantly better retention of encapsulated molecules when compared with DOPC phospholipid vesicles (Figure ). The percentage of the vesicles embedded in the gel was 18.6 v/v%. The 0.8% alginate solution mixed with EGTA-loaded vesicles was crosslinked with 50 mM CaCl2 solution (see Supporting Information). Figure shows that the vesicles were uniformly dispersed within the resulting hydrogel after crosslinking.