Alpha spectrometry is an indispensable technique in the radiology lab for the analysis of natural radionuclides. While the powerful ICP/MS is used more and more for the analysis of uranium and thorium, other radionuclides, such as 226 Ra, are difficult to analyze with this technique due to their very high specific activities. The following chapter is introduced by a description of the problems, which may occur when working in the ultra-trace level. A description of the commonly used extraction and enrichment techniques for alpha nuclides and a short survey of the commonly applied detection techniques are given. The main application of alpha spectrometry in our laboratory is the monitoring of tap and mineral waters. Besides water, some specific food categories, such as fish, seafood, spices or healing earths, are monitored for their content of natural radionuclides. Monitoring of Natural Radioactivity in Drinking Water and Food with Emphasis… DOI: http://dx.doi.org/10.5772/intechopen.90166 * Activity limits according to ordinance on drinking water and water for public baths and shower facilities (TBDV) [7].