Study of the state of equilibrium of any natural radioactive source requires determination of several key nuclides or groups of nuclides to find their contribution to the total amount of radioactivity. Alpha activity measured by scintillation counting is used for determination of protactinium-231, thorium-232, thorium-230, and radium-226. The chemical procedures for the separations of the specific elements are described, as well as the measurement techniques used to determine the abundances of the individual isotopes. To correct for deviations in the ore standards, an independent means of evaluating the efficiencies of the individual separations and measurements is used. The development of these methods of radiochemical analysis facilitates detailed investigation of the major sources of natural radioactivity.