Atomistic simulations of U-Zr fuel and its interaction with Fe, Ni, and Cr using the BFS method for alloys are presented. Results for the γU-βZr solid solution are discussed, including the behavior of the lattice parameter and coefficient of thermal expansion as a function of concentration and temperature. Output from these calculations is used to study the surface structure of γU-βZr for different crystallographic orientations, determining the concentration profiles, surface energy, and segregation behavior. The analysis is completed with simulations of the deposition of Fe, Ni and Cr on U-Zr substrates with varying Zr concentration. All results are discussed and interpreted by means of the concepts of strain and chemical energy underlying the BFS method, thus obtaining a simple explanation for the observed Zr segregation and its influence in allowing for cladding elements diffusion into the U-Zr fuel.