Al-substituted barium ferrite powders were synthesized using the sol-gel auto-combustion method according to the molecular formula BaAlxFe12−xO19 (x=0, 0.1, 0.2, 0.3, 0.4, 0.5, 1.0). Compared with non-substituted barium ferrite annealing at 1 000 ℃, the vibrating sample magnetometer (VSM) measurement manifested that the optimum magnetic properties formation temperature of Al-substituted barium ferrite was 1 100 ℃. The data from X-ray diffractometer (XRD) showed that with increasing x, the lattice constants (a and c) decreased as well as the unit-cell volume V cell . Magnetic measurement of non-substituted and Al-substituted powders annealed from 900 ℃ to 1 200 ℃ exhibited that the maximum magnetization M (10 kOe), the remanent magnetization Mr and the coercivity Hc depended strongly on the chemical composition of powder as well as the annealing temperature. When annealing at 1 100 ℃, BaAl0.5Fe11.5O19 of high coercivity Hc (6 584 Oe) was produced. Meanwhile, M (10 kOe) and Mr were 42.83 emu/g and 25.65 emu/g, respectively.