In many metallic alloys, complex microstructures form as a consequence of local atomic ordering that depends on the processing path. This research uses an atomistic approach to study microstructural morphology and evolution in order to investigate how temperature and alloy concentration affect ordering. A semi-empirical Modified Embedded Atom Method (MEAM) is used in conjunction with molecular dynamics (MD) and Monte Carlo (MC) simulations to investigate the properties and equilibrium configurations of the high temperature body-centered-cubic (bcc) uranium-zirconium (U-Zr) alloys. Atomic simulations conducted with the MEAM potential show the thermodynamic driving force to the lamellar structure for the melt-casted U-rich alloys and the finely acicular microstructure of the water quenched U-rich alloys. In addition, when the U-rich U-Zr alloy is equilibrated at a lower temperature, the lamellar/acicular microstructures begin to spheroidize, as observed in experiments. In the intermediate Zr concentration region, the ordering seen is able to facilitate the structure to the partially ordered δ-UZr 2 phase seen experimentally. Lastly, the Zr-rich region is able to successfully show the thermodynamic driving force to the acicular, Widmanstätten, and martensitic needles type microstructures observed experimentally. These simulations are able to successfully replicate some of the fundamental thermo-physical and microstructural characteristics following fabrication and irradiation of the U-Zr metallic fuels.