The Aluminums (Al) substituted on M-type barium ferrite (BaFe12O19) is one of the magnetic materials, which can be applied to the microwave band working at high frequencies. The purpose of this paper is to investigate the effect of Al substitution for Fe3+ ions on the structure, magnetic and absorption behavior of M-type barium ferrite. The sample was prepared by mechano-synthesis using high-energy milling (HEM). In this research, Fe ion in BaFe12O19 was substituted by Al ion to form BaFe12O19 for x = 0.0, BaFe12O19 for x = 2.0 and BaFe12O19 for x = 4.0 which is called as BAI-0, BAI-2 and BAI-4 sample, respectively. The stainless steel balls were used for the milling with a ball-to-powder sample ratio of 5. The mixing and milling for each the sample was conducted for 5 hours in ethanol medium and dried at 100 degrees C in oven for 24 hours and then followed by heat treatment at 1100 degrees C during 1 h in the atmosphere media. The sample was characterized using X-rays diffractometer (XRD), Scanning Electron Microscope (SEM), Vibrating Sample Magnetometer (VSM) and Vector Network Analyzer (VNA). The result indicates that the addition of Al ion lead to the change cell parameters, volume, and the particles size. The magnetic behavior such as magnetic coercivity (H-c), magnetization saturation (M-s) and remanent (M-r) changed significantly with the substitution of Al ions. The optimum reflection loss (RL) is found to be -35dB at 14GHz for BaFe12O19 (BAI-2) sample. It is shown that Al substitutions change the particle size, ferromagnetic resonant frequency, and structural and magnetic behavior of M-type barium ferrite.