Pure and D: alanina doped triglycin sulphate (TGS) crystals were grown from aqueous solutions. Fresh cleaved, polished and silver paste painted samples were temperature and frequency investigated. Pure crystals show nonreproducible values of the permittivity and dielectric loss crossing up and down the Curie point. More stable and much lower values of the permittivity and dielectric loss could be noticed for D: alanina doped crystals. Permittivity and loss values show different frequencies behavior related to polar or nonpolar state of crystals. Frequency dependence of permittivity and loss behavior could be related to the general picture of relaxation of different polarization mechanisms and their contributions to permittivity and loss values for dielectric materials. Much smaller and stable values of permittivity and loss, vs. temperature and frequency, were found for doped crystals. Experimental results point out for a more stable structure with dipoles mobility decreased of doped vs. pure TGS crystals. Thus, higher figure of merit of doped TGS crystals point to a major advantage for technical applications (© 2010 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)