Abstract: Biological systems are often assembled from flexible building blocks. Most computational studies of the assembly of bio-inspired soft materials focus on coarse-grained rigid building blocks. We present a study of the self-assembly of deformable building blocks using the virus capsid system as an example. A coarse-grained model of deformable capsomers that incorporates their stretching and bending energies is developed for a general small virus capsid system based on the building units of the minute virus of mice (MVM) capsid. Molecular dynamics simulations show that deformable capsomers can produce the rich assembly diagram associated with self-assembling capsid proteins including symmetric capsids and kinetically-trapped disordered structures. The pronounced effects of changing capsomer flexibility on the assembly behavior are discussed. In the second part of the talk, we address a key synthesis challenge in the design of multilayered bio-inspired soft materials by introducing a simple strategy to control the spatial arrangement of a mixed population of building blocks in a one-pot fabrication. Using coarse-grained simulations and SAXS experiments, we show that a mixture of two types of virus-like particles derived from bacteriophage P22, each type characterized by a distinct surface charge, selectively self-assembles into ordered core-shell structures in the presence of oppositely-charged dendrimers. The critical role of the ionic strength modulation and associated electrostatics-based control mechanism is highlighted.