In the present work, Al3+3+ substituted cobalt ferrites (CoFe2−x2−xAlxO4, x=0.2x=0.2, 0.4, 0.6, 0.8) have been synthesized via standard solid-state reaction technique. The incorporation of Al3+3+ ions in cobalt ferrite has been shown to play an important role in modifying the magnetic properties. The room temperature (300K) 5757Fe Mössbauer spectra reveals that the studied samples show two characteristic ferromagnetic zeeman sextets at A and B-sites at lower Al3+3+ ion concentration (i.e., up to x=0.4x=0.4). However, a paramagnetic relaxation has been noted for higher Al3+3+ substitution (for x=0.6x=0.6 and 0.8) samples. The dependence of the Mössbauer parameters such as isomer shift, quadrupole splitting, line width and magnetic hyperfine field on Al3+3+ ion concentration has also been noted. The variations in initial permeability over a wide frequency range (125kHz to 30MHz) at 300K have been recorded. The fairly constant values of initial permeability and the low values of the relative loss factor of the order of 10−4−4 to 10−5−5 over the wide frequency range are the important findings of the present work. The observed low values of relative loss factor at high frequencies suggest that the studied ferrites are promising materials to be used in microwave applications.