The quality of harvested rainwater which is used for domestic and drinking purposes in the northern area of Kefalonia Island in SW Greece and the factors affecting it were assessed through 3-year surveillance. In 12 seasonal samplings, 156 rainwater and 144 ground- or mixed water samples were collected from ferroconcrete storage tanks (300-1000 m3 capacity), which are adjacent to cement-paved catchment areas (600-3000 m2). Common anions and major cations as well as the metals Fe, Mn, Cd, Pb, Cu, Cr, Ni and Zn were tested. The presence of three major groups of organic compounds, polycyclic aromatic hydrocarbons (PAHs), organochloride pesticides (OCPs) and volatile organic compounds (VOCs), was screened by common analytical techniques. All of the rainwater samples were within the guidelines for chemical parameters established by the 98/93/EU directive. As far as microbiological quality is concerned, total coliforms, Escherichia coli and enterococci were detected in 80.3%, 40.9% and 28.8% of the rainwater samples, respectively, although they were found in low concentrations. Chemical and microbiological parameters showed seasonal fluctuations. Principal component analysis revealed that microbiological parameters were affected mainly by the cleanness level of catchment areas, while chemical parameters were influenced by the sea proximity and human activities. Disinfection should be applied into the tanker trucks which distribute the water to the consumers and not into the big storage tanks in order to avoid by-products formation. Due to the lack of fluoride in rainwater samples, the consumers must become aware of the fact that the supplementation of this element is needed.