Highly oriented Ge 0.81Sn 0.19 nanowires have been synthesized by a low-temperature chemical vapor deposition growth technique. The nanostructures form by a self-seeded vapor-liquid-solid mechanism. In this process, liquid metallic Sn seeds enable the anisotropic crystal growth and act as a sole source of Sn for the formation of the metastable Ge 1-xSn x semiconductor material. The strain relaxation for a lattice mismatch of ϵ = 2.94% between the Ge (111) substrate and the constant Ge 0.81Sn 0.19 composition of nanowires is confined to a transition zone of <100 nm. In contrast, Ge 1-xSn x structures with diameters in the micrometer range show a 5-fold longer compositional gradient very similar to epitaxial thin-film growth. Effects of the Sn growth promoters' dimensions on the morphological and compositional evolution of Ge 1-xSn x are described. The temperature- and laser power-dependent photoluminescence analyses verify the formation of a direct band gap material with emission in the mid-infrared region and values expected for unstrained Ge 0.81Sn 0.19 (e.g., band gap of 0.3 eV at room temperature). These materials hold promise in applications such as thermal imaging and photodetection as well as building blocks for group IV-based mid- to near-IR photonics.