The gross alpha and beta activity concentrations in the thermal waters of Karakaya-Ayas, Icmece-Ayas, Beypazar (Dutluk-Tahtali), Haymana, and Kizilcahamam spas in Ankara Province were measured by MPC-9604 multi-detector alpha/beta counting system. Ranges of activity concentrations found were from 0.09 to 2.58 Bq L-1 for gross beta and from 0.25 to 2.61 Bq L-1 for gross beta. The ranges of minimum detectable concentrations for gross alpha (0.05-0.41 Bq L-1) and for gross alpha (0.04-0.29 Bq L-1) were obtained. Gross alpha and beta activity concentrations found in samples were compared with the recommended guidelines of the World Health Organization and the Turkish Standards, and literature values. Na, K, Ca, Si, Mn, Ce, Te, Nd, Sm, Cs, W, La, U, and Th metal levels in these thermal ground waters were also determined by using wavelength dispersive X-ray fluorescence spectrometry (WDXRF).