range of rheological properties of capsulecontaining solutions that can be accessed; the formulation of capsule-based solutions displaying a pronounced shear thinning or a yield stress would be key to use them as 3D printable inks. Capsules with much thinner, flexible shells whose structure and surface composition can be varied over a wide range can be fabricated from emulsion drops by solidifying reagents at their surface. This can be achieved, if appropriate reagents are dispersed in the drop and complementary ones in the continuous phase. Once these reagents meet at the drop surface, they solidify through polymerization [21][22][23] or coacervation reactions. [24][25][26][27] Capsules with thin shells can also be produced from a single type of reagent, namely from chemically reactive surfactants, that are cross-linked at the drop surface. [28][29][30][31][32] However, the number of reagents that can be employed to form thin polymeric capsules through these approaches is limited. Flexible capsules that display a narrow size distribution, low permeability toward encapsulants, allow controlled exchanges of reagents, and are mechanically sufficiently stable to withstand significant shear stresses such that they can be processed into macroscopic materials through additive manufacturing techniques remain to be established. These capsules would open up a new field of their use as principal building blocks of macroscopic granular materials with well-defined micrometer-sized structures and locally varying compositions that go far beyond their current use as individually dispersed delivery vehicles.Here, we introduce a new type of viscoelastic, mechanically stable capsules that are composed of bioinspired ionically crosslinked catechol-functionalized block-copolymer surfactants. These capsules present Fe 3+ complexed catechols at their surface such that they have a high affinity to each other. Therefore, they cannot only be used as individually dispersed mobile carrier vehicles that enable triggered release of reagents, but also as principal building blocks of macroscopic soft materials. We demonstrate for the first time that these capsules are mechanically sufficiently stable to serve as principal building blocks of inks that can be 3D printed into macroscopic granular materials with well-defined micrometer-length-scale structures.Emulsion drops are often stabilized with polymeric surfactants that are crucial during drop production and storage. However, once the drops are converted into capsules, surfactants are usually superfluous or even devastating because they irreproducibly change the surface wettability of the Microcapsules are often used as individually dispersed carriers of active ingredients to prolong their shelf life or to protect premature reactions with substances contained in the surrounding. This study goes beyond this application and employs microcapsules as principal building blocks of macroscopic 3D materials with well-defined granular structures. To achieve this goal and inspired by nature, capsules ...