The pollution of the surface waters of Greece from the priority compounds of 76/464/EEC Directive was evaluated. The occurrence of 92 toxic compounds, 64 of which belong to priority compounds of List II, candidates for List I, of 76/464/EEC Directive, was studied in surface waters and wastewater through the developed network of 62 sampling stations, which covers the whole Greek territory. The analytical determination was performed by Purge and Trap-Gas chromatography-Mass spectrometry for volatile and semivolatile organic compounds (VOCs), Gas Chromatography-Electron Capture Detection for organochlorine insecticides, Gas Chromatography-Nitrogen Phosphorous Detection for organophosphorous insecticides, High Performance Liquid Chromatography-Photodiode Array Detection for herbicides, and Electrothermal Atomic Absorption Spectrophotometry and Inductively Coupled Plasma-Atomic Emission Spectrometry (ICP-AES) for metals and the toluene extractable organotin compounds. The concentrations of VOCs and insecticides detected in the surface waters of Greece were very low, whereas the concentrations of herbicides and metals ranged generally at moderate levels. VOCs were detected almost exclusively in the rivers and very rarely in the lakes, while the frequency of occurrence of insecticides, herbicides and metals was similar for rivers and lakes. Water quality objectives (WQO) and emission limit values (ELV) have been laid down in national legal framework for a number of compounds detected in the samples, in order to safeguard the quality of surface waters from any future deterioration.