This paper presents measurements of the effect of the atmospheric radioactive release from the Fukushima Dai-ichi nuclear power station at three sites belonging to the Spanish environmental monitoring system. Measured values varied depending on the locations of the sites in Spain and their respective climatic characteristics. 134Cs, 136Cs, 137Cs, 131I, and 132Te activity concentrations in filter samples were studied and associated levels of 131I fallout were estimated from wet and dry deposition. Particulate aerosol activity concentrations ranges, in mBq/m3, were 1.63e3080 (131I), 2.8e690 (137Cs), 1.3e620 (134Cs) and 3.6e330 (132Te), while the associated 131I fallout was roughly estimated to be less than 20 Bq/m2, Gaseous 131I was also detected and the 131I-gaseous/131I-total ratio increased at the three stations from approximately 0.75 at the end of March to 0.85e0.9 during the first few days of April. Finally, the presence of 131I in some crucial parts of the food chain was also studied. 131I was detected in samples from goat’s and cow’s milk (maximum levels of 1.11 Bq/L) and in broadleaf plants (maximum level 1.42 Bq/kg).