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3D bioprinting additively assembles bio‐inks to manufacture tissue‐mimicking biological constructs, but with the typical building blocks limited to 1D filaments. Here, it is developed a voxelated bioprinting technique for the digital assembly of spherical particles (DASP), which are effectively 0D voxels—the basic unit of 3D structures. It is shown that DASP enables on‐demand generation, deposition, and assembly of viscoelastic bio‐ink droplets. A two‐parameter diagram is developed to outline the viscoelasticity of bio‐inks required for printing spherical particles of good fidelity. Moreover, a strategy is developed for engineering bio‐inks with independently controllable viscoelasticity and mesh size, two of the most important yet intrinsically coupled physical properties of biomaterials. Using DASP, mechanically robust, multiscale porous scaffolds composed of interconnected yet distinguishable hydrogel particles are created. Finally, it is demonstrated the application of the scaffolds in encapsulating human pancreatic islets for sustained responsive insulin release. Together with the knowledge of bio‐ink design, DASP might be used to engineer highly heterogeneous, yet tightly organized tissue constructs for therapeutic applications.

Properties of emulsions highly depend on the interdroplet interactions and, thus, engineering interdroplet interactions at molecular scale are essential to achieve desired emulsion systems. Here, attractive Pickering emulsion gels (APEGs) are designed and prepared by bridging neighboring particle‐stabilized droplets via telechelic polymers. In the APEGs, each telechelic molecule with two amino end groups can simultaneously bind to two carboxyl functionalized nanoparticles in two neighboring droplets, forming a bridged network. The APEG systems show typical shear‐thinning behaviors and their viscoelastic properties are tunable by temperature, pH, and molecular weight of the telechelic polymers, making them ideal for direct 3D printing. The APEGs can be photopolymerized to prepare APEG‐templated porous materials and their microstructures can be tailored to optimize their performances, making the APEG systems promising for a wide range of applications.