In this paper, the microstructure and dielectric properties of ion-doped La 0.7 Sr 0.3 MnO 3 are investigated in detail. The polycrystalline ceramics of La 0.7 Sr 0.3 Mn 1Ày M y O 3 (M ¼ Fe, Ni, Cu; y ¼ 0.3 or 0.5) are prepared by the sol-gel/sintering method. The symmetry of the crystal structure is improved and the dielectric properties obtained in the frequency range from 80 MHz to 1 GHz can be tuned by the doping of Fe, Ni, and Cu ions. With regard to the dielectric properties in lossy ceramics, the decrease of real permittivity 3 0 r for the doping of Fe and Ni will be effective for impedance-matching; the enhanced dielectric losses in the Ni and Cu doping samples will promote stronger absorption. Thus, the improved dielectric properties make ion-doped La 0.7 Sr 0.3 MnO 3 promising candidates for lossy ceramics in microwave electronics. In addition, the experimental results of permittivity were checked by K-K relations, and the frequency dispersion behaviors of the conductivity within a certain frequency range accord with the Jonscher's power law in the form of s 0 ac (f) f (2pf) n , demonstrating that the conductive mechanism is hopping conduction.