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Alkali tantalates are encouraging functional materials with versatile properties that make them potential players in microelectronics, photocatalytic processes or medicine. Here, KTaO₃ single crystals with 0.27% Li and 0.15% or 0.31% Mn contents determined by inductively coupled plasma spectroscopy analysis are studied at low temperatures using dielectric spectroscopy in a frequency range of 10²–10⁶ Hz. Both Li and Mn doping are found to induce separate low-frequency dielectric relaxations of comparable strength in KTaO₃. The relaxation dynamics follow the Arrhenius law with activation energy values of ~77 and 107 meV, attributing the relaxation origin to the dipoles formed by off-centre Li⁺_K and Mn²⁺_K ions, respectively.