This study aimed to estimate the radiofrequency exposure levels in the vicinity of nursery and primary schools at the northwest part of Crete island in Greece. Moreover, the compliance with the exposure limits, according to Greek legislation, was investigated. A total of 396 in situ frequency-selective and broadband measurements were conducted around 69 schools, classified in urban and suburban environments, in the range of 27–3000 MHz (subdivided in seven frequency bands). The measured value of the electric field strength (V/m) was recorded and, subsequently, the exposure ratio was calculated. Statistical analysis was performed in order to analyze and evaluate the data. In addition, a worst-case scenario was examined by considering the highest measured exposure level around each school. The statistical tests indicated that the mean and median values of the exposure ratio, even in the worst-case scenario, were found well below 1 for all frequency bands. The calculated distributions of the electric field measurements demonstrated that almost 90% of the latter were below 1 V/m, with the majority of values lying in the range of 0.5–1 V/m. The main contributors to the total exposure were the mobile communication frequencies and broadcasting, while the exposure was greater in urban than in suburban environments.