Airborne Volatile Organic Compounds (VOCs) play an important role in the atmospheric chemistry which leads to an increase in the formation of ozone and photochemical oxidants that are harmful to human health and ecosystem. In this work, VOCs were monitored in Ethiopia at two different cities (Jimma and Addis Ababa) through 2 sampling campaigns conducted in the period between August to September 2010. Active sampling was used on sorbent tubes filled with Tenax TA. The analysis was done by TD-GC-MS using internal standard calibration. This work has brought forward new data on 34 VOCs concentration levels (mig/m3) of 2 urban sites in Ethiopia. This is the first investigation of concentration levels of VOCs in the urban air environment of Ethiopia.