The results of dielectric properties and direct current specific electric conductivity measurements in Armenian natural clinoptilolite samples are presented. Electron irradiation with energy 8 MeV and thermal treatment of samples are performed to elucidate possible enhancement mechanisms of clinoptilolite parameters. The results are discussed on the basis of new point structural defects formation and recombination of initial ones in samples. It was shown that the irradiation dose of 3·1016 el/cm2 is critical for natural zeolite structural change, which is manifested by significant changes in dielectric properties and other characteristics. The samples subjected to high temperature heating after electron irradiation, in comparison with an unquenched one, have a significantly higher (about an order of magnitude) value of specific conductivity.