Vanadium titanomagnetite is an important mineral resource. It is a raw material for ironmaking, vanadium extraction, strategic metal titanium production, and titanium dioxide production. In this study, high chromium vanadium titanomagnetite (High-Cr VTM) and ordinary iron ore were used as raw materials for pelletizing. The effect of V2O5 on the preparation and properties of High-Cr VTM pellets was studied. The influence of V2O5 on the properties of the green pellets, the compressive strength of oxidized pellets, the reduction swelling index and reduction degree, softening-melting behavior, and the migration law of Fe, Ti, and Cr in the reduction process were studied by X-ray diffraction (XRD) and scanning electron microscopy (SEM). The results show that with the increase in V2O5 content, the properties of the green pellets basically showed a trend of first decreasing and then increasing but all met the basic requirements of pelletizing. When the added amount of V2O5 in the pellet was 6%, the compressive strength of the oxidized pellet was the lowest at only 2565 N/pellet but it still met the quality requirements for pellets in blast furnace production. As the dosage of V2O5 increased, the reduction swelling index and reduction degree of the pellets showed a trend of first increasing and then decreasing. The addition of V2O5 can increase the softening initial temperature, softening final temperature, melting start temperature, and dripping temperature of the High-Cr VTM pellets, narrowing the softening interval, and expanding the melting dripping interval. The experimental results provided a data reference for revealing the influence of V2O5 on High-Cr VTM pellets during the blast furnace smelting process.