The elemental segregation behaviors and interactions between point defects and symmetrical tilt grain boundaries (GBs) in TiVTa concentrated solid–solution alloys (CSAs) have been studied through hybrid Monte Carlo/molecular dynamics (MC/MD) simulations. A pure V model, a random TiVTa CSA with randomly distributed elements, and an equilibrated TiVTa CSA with Ti segregation were constructed to investigate the influence of chemical disorder and local elemental segregation on defect–GB interactions. For defect–GB interactions, GBs interact more strongly with interstitials than with vacancies. Compared with the pure V, the vacancy absorption length scale of GBs is greater, whereas the interstitial absorption length scale of GBs is shorter in TiVTa CSAs due to the chemical fluctuation and local lattice distortion. This means a higher recombination efficiency of point defects in TiVTa CSAs. The elemental (Ti) segregation in TiVTa CSAs can further enhance the sink strength of GBs towards interstitials, while simultaneously reducing their sink strength towards vacancies. Consequently, the preference effects of GBs towards interstitials and vacancies are amplified in the equilibrated CSA due to local ordering, thereby reducing efficient defect annihilation around GBs. These results provide fundamental insights into the irradiation defect dynamics of CSAs with body-centered cubic (bcc) structure.