In this study, the correlations between the shrinkage behavior, densification mechanism, and atomic diffusivity of the atomized and milled Ti-based crystalline alloy powders are investigated. The densification mechanism of each stage was identified by determining the evolution of the characteristic microstructures at different sintering temperatures in combination with the shrinkage behavior. Importantly, a theoretical framework is established here and elaborate how it can be used to determine the value of the atomic diffusivity DT and a factor g by integrating the interior (related to material properties) and exterior (related to the sintering parameters) variables. This approach can be utilized to provide insights into the active densification mechanisms during spark plasma sintering (SPS). Furthermore, the densification behavior and microstructure evolution of the two types of heat-treated Ti-based alloy powders fabricated by gas atomization and ball milling are compared to validate the framework for different pressures (15, 30, 45, and 60 MPa) and heating rates (30, 60, 90, and 120 K/min). The results indicate that the comprehensive factor g and the atomic diffusivity DT can be used to describe the densification mechanism and thus the shrinkage behavior during each densification stage. Our results provide quantitative proof that the applied pressure and heating rate promote diffusivity to accelerate powder densification during SPS.