The aim of the present work was to compare the results obtained with gross alpha methods such as evaporation, co-precipitation and total evaporation by liquid scintillation counting and to check whether these results are representative of the real total alpha activity concentration on the sample. The study was carried out on eight natural waters with very different radioactive characteristics. For all the samples uranium ( 238 U, 235 U, and 234 U), radium ( 226 Ra and 224 Ra), 210 Po, and 232 Th isotopes were also assayed by using radiochemical separation and alpha spectrometry in order to determine the sum of the activities of these alpha emitters. Precision (expressed as relative standard deviation) was below 28% for evaporation and below 18% for co-precipitation. In the case of total by liquid scintillation counting it was below 10% for samples with Total Alpha activity above 0.1 Bq/L (this value is about three times the MDA). Furthermore, for most of the studied waters, the Total Alpha activity and the gross alpha activity determined by the three methods were comparable. The obtained bias by the evaporation, co-precipitation, and total evaporation by liquid scintillation counting methods was lower than 40%, 25% and 20%, respectively. The ANOVA test was applied to fi nd out if there was signi fi cant variability among the methods. For the samples with the most common radiochemical characteristics there were no signi fi cant differences among the three studied methods. However differences were detected for samples with a high saline content or with a very low activity level.