The permittivity components of the liquid crystalline gadolinium complex with Lewis bases and β-diketonates as ligands are measured in the frequency range from 100 Hz to 5 MHz. The magnitude and sign of the dielectric anisotropy of the complex are determined. Two dispersion regions of the permittivities are found in the liquid crystalline phase. The mechanisms responsible for the relaxation phenomena occurring in the sample are established. The dielectric relaxation times, activation energies, and dipole moment of the complex are obtained. The results of the study are compared with the dielectric properties of ytterbium and terbium complexes having the same ligand environment.