The present invention generally relates to a method and apparatus to produce and apply a variety of surface cleaning and modification spray treatments. More specifically, the present invention provides the simultaneous steps of selectively removing one or more unwanted surface contaminants, including extremely hard coatings, exposing a native clean surface layer and modifying said exposed and cleaned native substrate surface layer to energetic radicals and radiation to improve adhesion, wettability or coatability. Reactive species in combination with non-reactive, but chemically or physically active, species provide a reaction control and surface treatment environment by which contaminants and surface interlayers are oxidatively, physically and/or chemically removed or modified to prepare an underlying substrate surface for subsequent bonding, deposition, coating and curing operations. Substrates treated in accordance with the present invention have cleaner and higher surface free energy surfaces.