An analytical method for simultaneous determination of "particle"-associated and "gaseous"-phase concentrations of polychlorinated biphenyls (PCB) and polycyclic aromatic hydrocarbons (PAH) in atmospheric aerosol samples obtained by high-volume samplers using polyurethane foam adsorbent (PUF) and quartz fibber filters (QFF) has been investigated. Quality control of the analytical procedure was carried out by blank control and by evaluating limits of detection, recoveries, accuracy, and repeatability. The proposed method was subsequently used to determine PAH and PCB in the "gaseous" and "particulate" phases of the aerosols that enter the Venice Lagoon atmosphere. The highest concentrations of sigma PCB and sigma PAH were predominantly in the "gaseous" phase. In both "particulate" and "gaseous" phases the penta-CB congeners dominated total PCB concentrations whereas phenanthrene, fluoranthene, and pyrene dominated the sigma PAH concentrations. Total ("gaseous" plus "particulate") PCB and PAH concentrations were higher at the site directly influenced by the industrial plants but the concentrations in marine aerosol samples were lower by a factor four only and must be taken into consideration when studying the chemical contamination of the Venice Lagoon.