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Abstract Recent advances in semiconductor based electronic devices can be attributed to the technological demands of ever increasing, application specific markets. These rapidly evolving markets for devices such as displays, wireless communication, photovoltaics, medical devices, etc. are demanding electronic devices that are increasingly thinner, smaller, lighter and flexible. High-quality, III-V epitaxial thin-films deposited on single-crystal substrates have yielded extremely high-performance, but are extremely expensive and rigid. Here we demonstrate heteroepitaxial deposition of GaAs thin-films on large-grained, single-crystal-like, biaxially-aligned, flexible, metallic substrates. We use molecular beam epitaxy (MBE) for the controlled growth of high quality GaAs layers on lattice matched Ge capped, flexible metal substrates. The structural, optical, interfacial and electrical characteristics and properties of the heteroepitaxial GaAs layers are analyzed and discussed. The results show that heteroepitaxial GaAs layers with good crystalline and optoelectronic properties can be realized for flexible, III-V based semiconductor devices. III-V materials integrated on large-grained, single-crystal-like, flexible, metallic substrates offer a potential route towards fabrication of large-area, high-performance electronic devices.