Long half-life natural and artificial radionuclides have been paid great attention in the environment, geochronology, nuclear accidents, as well as the operation of nuclear facilities for over a decade. However, the rapid and accurate quantification of these ultra-trace level (fg or mBq) radionuclides has become a formidable challenge nowadays. A triple-quadrupole inductively coupled plasma mass spectrometry (ICP-MS) equipped with a collision reaction cell (CRC), namely ICP-MS/MS, is a valuable technique for rapid and sensitive analysis of ultra-trace level radionuclides in various kinds of samples. This article provides a comprehensive review and critical comparison of published analytical methods for ultra-trace level radionuclides in environmental, biological and nuclear waste samples. The methods of sample pre-treatment, valence state adjustment, chemical separation of radionuclides, and ICP-MS/MS measurement are systematically described and discussed. Importantly, the advantages and limitations of the collision reaction cell (CRC) technology on the removal of interferences and the radionuclide measurement are comprehensively summarized. In addition, the article also explores advancements in automated separation and measurement methodologies for radionuclides.