Three methods for determination of alpha-emitting nuclides using liauid scintillation counting are compared, and the pertinent literature is reviewed. Data showing the application of each method to the measurement of plutoniura concentration in tissue and bone samples are presented. Counting with a commercial beta-liquid scintillation counter and an aqueous-phase-accepting scintillator is shown to be accurate only in cases where the alpha activity is high (several hundred counts/min or more), only gross alpha counting is desired, and beta-ganuna emitters are known to be absent from the sample or present at low levels compared with the alpha activity. Counting with the same equipment and an aqueous imrciscible scintillator containing an extractant for the nuclide of interest (extractive scintillator) is shown to allow better control of alpha peak shift due to quenching, a significant reduction of betagamma interference, and, usually, a low background. The desirability of using a multichannel pulse-height analyzer in the above two counting methods is stressed. The use of equipment and procedures designed for alpha liquid scintillation counting is shown to allow alpha spectrometry with an energy resolution capability of 200 to 300 keV full-peakvridth-at-half~peak-height and a background of 0.3 to 1.0 counts/min/,' or as low as 0.01 counts/min if pulse-shape discrimination methods are used. Methods for preparing animal bone and tissue samples for assay are described.