The hetero- and homoepitaxial deposition of GaAs films by the ionized cluster beam technique in connection with subsequent neutral beam deposition forming a double layer structure have been studied. It is found that ICE-deposited films have superior quality in comparison with conventional ion beam deposited films and comparable quality like MBE or MOCVD-deposited films. By the fabrication of device structures, it has been proved that the start of film growth from an interface formed by an ICE-deposited As layer is advantageous. Additionally, surface cleaning by low-energy ionized cluster beams has been studied. For the first time, defect-free surface cleaning by low-energy cluster ion beams has been realized.