Insights into material structures and properties from novel computational approaches have the potential to advance technologies and address critical challenges in a wide variety of fields ranging from photonics to healthcare to environmental sustainability. In materials discovery and development, two critical knowledge gaps remain: elucidating the relationship between the chemical building blocks and the structures they form, and the connection between structures and the corresponding properties they exhibit. In this talk, I will present examples from my prior research which have addressed these gaps. First, I will discuss the use of chemistry-agnostic models to examine the self-assembly of nanoparticles into colloidal crystals in both two and three dimensions, in systems mimicking both metallic alloys and salts. I will examine the influence of increasingly disparate particle size on the stability of mixed, bcc-type crystals using a tunable particle–particle interaction model. Second, I will elucidate the failures of equilibrium molecular dynamics to capture the viscous behavior of some complex solutions and discuss the implementation of a novel pathway for estimating the shear viscosity of structured liquids via non-equilibrium all-atom molecular dynamics and demonstrate its efficacy using lauramidopropyl betaine/sodium dodecyl sulfate micellar fluid as a case study.