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In this study, the effects of spinodal decomposition on the microstructures and mechanical properties of a TiZrNbTa alloy are investigated. The as-cast TiZrNbTa alloy possesses dual phases of TiZr-rich inter-dendrite (ID) and NbTa-rich dendrite (DR) domains, both of which have a body-centered cubic (BCC) structure. In the DRs of the as-cast alloy, the α and ω precipitates are found to be uniformly distributed. After homogenization at 1100 °C for 24 h followed by water quenching, spinodal decomposition occurs and an interconnected structure with a wavelength of 20 nm is formed. The α and ω precipitates remained in the structure. Such a fine spinodal structure strengthens the alloy effectively. Detailed strengthening calculations were conducted in order to estimate the strengthening contributions from the α and ω precipitates, as well as the spinodal decomposition microstructure.