Polymer matrix composites based on ED-20 epoxy resin, hollandite K1.6(Ni0.8Ti7.2)O16 and carbon nanotubes with a variable content of 0.107; 0.213 and 0.425 vol.% were obtained for the first time. Initial components and composites produced were characterized by XRD, XRA, FTIR, SEM and Raman spectroscopy. The dielectric properties of composite materials were measured by impedance spectroscopy and determined by the volume ratio of the composite components, primarily by the concentration of CNTs. At a CNT content of 0.213 vol.% (before percolation threshold), the maximum synergistic effect of carbon and ceramic fillers on the dielectric properties of a composite based on the epoxy resin was found. Three-phase composites based on epoxy resin, with a maximum permittivity at a minimum dielectric loss tangent, are promising materials for elements of an electronic component base.