Segregation defects greatly affect the service performance and working life of castings during the vacuum arc remelting (VAR) process. However, the corresponding research on the prediction of segregation defects is still not comprehensive. Through considering the influence of water-cooled crucible on the electromagnetic field inside an ingot, a full-scale model for the comprehensive prediction of freckles and macrosegregation defects during the VAR process is developed in this paper. The macroscopic solute transport phenomenon and the segregation behavior of Ni-5.8 wt% Al-15.2 wt% Ta alloy are predicted. The results indicate that the freckles are mainly concentrated in the lower region of the ingot. With the growth of the ingot, the solute enrichment channels gradually develop into solute enrichment regions, and the channel segregation evolves into macrosegregation. The Lorentz force mainly affects the flow pattern at the top of the molten pool, while the complex flow of multiple vortices is dominated by thermosolutal buoyancy. The maximum and minimum relative segregation ratio inside the ingot can reach 290% and −90%, respectively, and the positive segregation region accounts for about 79% of the total volume. This paper provides a new perspective for understanding the segregation behavior inside the ingot by studying the segregation evolution during the VAR process.