A series of spinel ferrites Mn0.5-xNixZn0.4Cu0.1Fe1.95Al0.05O4 have been prepared by auto-combustion technique. X-ray diffraction (XRD) and Field Emission Scanning Electron Microscopy (FESEM) have been used for structural and morphological investigations. The XRD patterns confirm the formation of cubic spinel structure of ferrites. The lattice constants decrease with the increase of Ni contents due to the smaller ionic radii of Ni2+ compared to Mn2+ as well as particle size decreases. Density is increased and porosity is decreased with the increase of Ni contents in the samples due to the higher atomic weight of Ni2+ compared to Mn2+. The FESEM analysis reveal that the average size of the irregularly shaped grains increased with Ni contents. The mixed spinel structure is further confirmed by the FTIR spectra, which show a doublet band at about 600 cm−1. The observed optical band gap and the particle size variations are comparable, and the quantum size effect supports this conclusion. The real part of initial permeability and relative quality factor increase with the increase of Ni contents due to increase of density and grain size as well as decrease of porosity. Also, it is found that magnetic loss decreased with the increase of Ni contents. All the samples exhibit ferrimagnetic behavior and the number of Bohr magneton has been calculated for all compositions. The dielectric constant shows large value in the lower frequencies and decreases with frequency shows dispersion due to Maxwell-Wagner space charge polarization. The investigation of electric modulus has demonstrated the existence of the hopping conduction mechanism. The AC conductivity is very low at lower frequency region and very large at higher frequency region which can be explain according to the polaron hopping model of Austin and Mott. The AC conductivity enhances nearly linearly with frequency, suggesting that the mechanism of conduction is due to small polaron hopping, which can be described according to Jonscher’s power law. Also, the effect of grain and grain boundary resistance on transport properties has been investigated using complex impedance analysis and it has been observed that both exhibit an increase trend as the Ni content increases.