22 sludge samples were analyzed from three municipal wastewater treatment plants to assess both the occurrence and the temporal behavior of radioactivity during 8 sampling campaigns carried out over the period 2007–2009. As regards natural gamma emitters radionuclides from the natural 238U series (such as 234Th, 214Pb, 214Bi, 210Pb) and the 232Th series (such as 228Ac, 212Pb, 212Bi and 208Tl) and other natural gamma emitters such as 7Be, 210Pbu or 40K were measured. In the case of man-made radionuclides small amounts of 137Cs were found, while significant amounts of 131I were detected in some samples. Correlations were found between radionuclides with the same origin. No seasonal variation for the 238U and 232Th series was found in the studied period but 7Be and 210Pbu showed seasonal variation that was explained by the monthly rainfall. The internal and external hazard indices were calculated and the results indicate that the radiological characteristics of the sludge do not present a significant radiological risk and make them suitable for future applications.