Analogues of pixels in two-dimensional (2D) pictures, voxels –– in the form of small cubes or spheres –– are the basic units of three-dimensional (3D) objects. Digital assembly of bio-ink voxels may provide an approach to engineering heterogeneous yet tightly organized 3D tissue mimics. However, this approach requires precisely manipulating highly viscoelastic bio-ink voxels in 3D space, which represents a grand challenge in both soft matter science and biomanufacturing. In this talk, I will introduce a voxelated bioprinting technology that enables the Digital Assembly of Spherical bio-ink Particles (DASP). First, I will discuss the criteria and nonlinear rheology for the on-demand generation, disposition, and assembly of viscoelastic bio-ink droplets in an aqueous environment without the help of large interfacial tension. Second, integrating software and hardware engineering, I will describe how to use DASP to create multi-material 3D structures consisting of interconnected, yet distinguishable particles made of different bio-inks. In parallel, I will show how polymer science can be used to guide the design and synthesis of modular, cell-instructive bio-inks suitable for voxelated bioprinting. Finally, I will share our recent progress in applying DASP for basic and translational biomedicine: (i) encapsulating islets into multiscale porous scaffolds to treat type 1 diabetes, and (ii) printing multi-material structures for probing heterotypic cell-cell interactions in 3D angiogenesis. I will also discuss emerging opportunities and challenges associated with voxelated bioprinting.