During three measuring campaigns in June, July, and August 1996, volatile organic compound (VOC) concentrations were measured at a rural background site, a city residential site, and a street site in Berlin. In addition, samples were taken near relevant sources of VOCs. The measurements covered the volatile hydrocarbons in the range C1-C14 and included aldehydes and ketones. Samples were taken at four characteristic periods of 2 hr/day: during the night, during the early morning rush hour, at midday, and during the evening rush hour. An assessment of the contribution of emission categories to the observed concentrations was made with the chemical mass balance (CMB) modelling technique. The VOC concentrations at the residential area and at the street site in the inner city were, respectively, a factor of 3 and 7 above the background concentration. Traffic exhaust contributed approximately 80-90% of the non-methane hydrocarbon (NMHC) concentration in the inner city and approximately 60% at the background area. Evaporative losses of motor fuel are estimated to account for approximately 7% at all sites. Natural gas leakage also contributed significantly to the observed VOC concentrations: in the inner city approximately 510% and at the background area approximately 30%. The measurements also showed a contribution of smaller sources, such as dry cleaning, use of solvents, and biogenic emissions. However, the contribution of these sources to the total observed concentrations at the sites is estimated to be very small.