Setting times, as the early-age properties of cement-based materials, are important properties to ensure the quality and long-term performance of engineering structures. To determine the initial and final setting times of cementitious materials, the compressive wave velocity and shear wave velocity of six early-age mortar samples were monitored. Their time evolution curves of Young's modulus, shear modulus, bulk modulus, and Poisson's ratio were then calculated and analyzed. The signature times of the derivatives of the Poisson's ratio evolution curves correlate well with the initial and final setting times, and the remarkably high coefficient of determination values relative to the data from this study are higher than those presented in the current literature. The proposed derivative method on the Poisson's ratio evolution curve is as good as the derivative methods from vs. evolution curves used by prior studies for the estimation of both the initial and final setting times of the early-age properties of cement-based materials. The formation and subsequent disappearance of ettringite of low Poisson's ratio were postulated to cause the initial dip in the Poisson's ratio evolution curves.