The invention relates to a method for preparing high-alkalinity chromium-containing vanadium-titanium pellets by adopting calcium oxide. The method comprises the following steps of mixing the raw materials including vanadium titano-magnetite, additive calcium oxide powder and sodium bentonite, so that the alkalinity of the raw materials is 1.8 to 2.1, drying and drying respectively, and carrying out dry mixing and mixing; averagely distributing the mixed ore materials into two parts, adding water accounting for 3% to 4% of the total mass of the raw materials in the first part, adding water with the total mass of 6% to 8% of the total mass of the raw materials in the second part, uniformly mixing, and hermetically standing; when pelletizing is carried out, a first part of mineral powder isused in the forming period of the master ball, a second part of mineral powder is used in the growth period of the master ball, the water spraying amount before the growth of the master ball is controlled to be 1ml of 10g of ore powder to 2ml of 10g of ore powder of mineral powder, preventing adhesion between the master balls, and adding water for 40 seconds to 90 seconds at each time, so that thediameter of the prepared pellets ranges from 8mm to 12mm; and preparing raw ball braised material, drying, pre-xidizing and roasting, carrying out secondary high-temperature oxidation roasting to obtain high-alkalinity chromium-containing vanadium-titanium pellets.