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A facile and flexible approach is developed for controllable fabrication of novel multiple-compartmental calcium alginate capsule membranes with combined co-extrusion minifluidic devices for isolated co-encapsulation and synergistic release of diverse incompatible components.The multi-compartmental capsules exhibit distinct compartments, each of which is covered by a distinct part of a heterogeneous membrane.The volume and number of multiple compartments can be well-controlled by adjusting flow rates and device numbers for isolated and optimized encapsulation of different components;while the composition of different part of the heterogeneous membrane can be individually tailored by changing the composition of droplet template for flexibly tuning the release behavior of each component.Such a heterogeneous membrane provides more flexibilities for synergistic release with controllable release sequence and release rates to achieve advanced and optimized synergistic efficacy.The multi-compartmental capsule membranes show high potential for applications such as drug co-delivery, confined reactions, enzyme immobilizations, and cell cultures.