The high cost of single-crystal III–V substrates limits the use of gallium arsenide (GaAs) and related sphalerite III–V materials in many applications, especially photovoltaics. However, by making devices from epitaxially grown III–V layers that are separated from a growth substrate, one can recycle the growth substrate to reduce costs. Here, we show damage-free removal of an epitaxial single-crystal GaAs film from its GaAs growth substrate using a laser that is absorbed by a smaller band gap, pseudomorphic indium gallium arsenide nitride layer grown between the substrate and the GaAs film. The liftoff process transfers the GaAs film to a flexible polymer substrate, and the transferred GaAs layer is indistinguishable in structural quality from its growth substrate.