Three analytical techniques are presented which are used at PSI for determination of U and Th isotopes (234U, 235U, 238U, 228Th, 230Th, 232Th) in different materials, i.e. environmental samples (soils, minerals) and dental ceramics as well as in urine for in vitro monitoring of potentially exposed workers. Depending on the sample quantity available and/or required detection limits the measurements are performed either directly via gamma spectrometry or via alpha particle counting with preceding separation chemistry. The separation methods applied are based on either extraction chromatography or on sorption of U and Th on actinide selective resin. Following sample digestion, chemical yield spike additions (232U, 225Th or 225Th), chemical purification and electro-depositional source preparation, alpha particle measurement is carried out using low-level alpha spectrometry. This technique allows detection limits of less than 0.2 mBq per counting source if the assay lasts over a few days and is therefore suitable for determination of trace quantities of short-lived 225Th that can be hardly detected by means of mass spectrometric techniques.