With the decrease of high quality iron ore resources at home and abroad, the mass fraction of Al₂O₃ in pellets raw materials will become higher and higher, which may directly affect the balling property, pellets' roasting performance and product quality of iron concentrates. In this paper, a Brazilian hematite concentrate is used as raw material, and the mass fractions of Al₂O₃ in the pellets are adjusted to 1.0%, 2.0% and 3.0% by adding different types of aluminum-containing additive powders (pure alumina, hercynite, gibbsite and kaolinite) to investigate the effect law of aluminum occurrence state and mass fraction on the balling property and pellets' roasting behavior of hematite concentrate. The results show that both kaolinite and gibbsite significantly improve the falling strength of fresh pellets, and hercynite significantly increases the bursting temperature of fresh pellets; the compressive strength of roasting pellets decreases significantly when alumina and gibbsite are added; while the addition of kaolinite helps to improve the compressive strength of roasting pellets when the mass fraction of Al₂O₃ is below 2%; in general, the increase in the mass fraction of Al₂O₃ is unfavorable to the reduction of pellets, but can inhibit the reduction expansion to a certain extent; the influence of different aluminum occurrence state is different, among which kaolinite has the most obvious influence; from the analysis of ore phase, no obvious liquid phase is generated when alumina, hercynite, gibbsite are added, while more slag phase is generated when kaolinite is added. The consolidation of the pellets is further strengthened and the distribution of the introduced aluminum in the pellets is also more uniform.