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The diffusion behavior and phase equilibria in the Cu-Zn binary system were investigated using solid-solid and solid-liquid diffusion couples. Heat treatments at temperatures ranging from 100 to 750 °C were performed and the samples were examined using optical microscopy, energy dispersive x-ray spectroscopy, and electron probe microanalysis to identify the phases and to obtain composition profiles. Solubility limits of both solid solution and intermetallic phases were then evaluated, and a forward-simulation analysis (FSA) was applied to extract interdiffusion coefficients. The composition profiles from Hoxha et al. were also re-analyzed using FSA to obtain more reliable diffusion coefficient data without the assumption of constant diffusion coefficients for the intermetallic phases. A comprehensive assessment of the interdiffusion coefficients in three intermetallic phases of the Cu-Zn system was performed based on the results from the current study as well as those in the literature. Activation energies and Arrhenius pre-factors were evaluated for each phase as a function of composition. The fitted equations based on the comprehensive assessment have the capabilities of computing the interdiffusion coefficients of each of the phase at a given composition and temperature. Suggested modifications to the Cu-Zn binary phase diagram were presented based on the new experimental information gathered from the present study. A clear explanation is provided for the puzzling low Zn concentrations often observed in the Cu-rich fcc phase of Cu-Zn diffusion couples in comparison with the expected high solubility values based on the equilibrium Cu-Zn phase diagram.