In recent years, Ge and Ge 1−x Sn x materials and devices have achieved rapid progress in integrated photonics. However, conventional heteroepitaxy of active photonic devices compromises the area on Si for CMOS electronics, limiting the scale of integration. Furthermore, it is not possible to grow GeSn epitaxially on amorphous and/or flexible substrates toward 3D photonic integration in mid-infrared (MIR) regime. Here, we present low-temperature crystallization of direct bandgap, high crystallinity Ge 1−x Sn x (0.08 < x < 0.26) on amorphous dielectrics insulators (GeSnOI) toward 3D and flexible MIR integrated photonics. Utilizing eutectically-enhanced crystallization (EEC), an extraordinarily large average grain size of ∼100 µm has been achieved in blanket GeSn films crystallized on SiO 2 layers, flexible glass, and polyimide substrates alike. Furthermore, using Sn nanodot enhanced composition enhancement (NICE), we have achieved an average Sn composition as high as 26 at.% to further extend the optical response of GeSn toward λ = 3-5 µm. The achieved Sn composition of 8-26 at.% far exceeds that of the equilibrium solubility limit of <1 at.%, even though the crystallization temperature of 350-450 • C far exceeds the typical epitaxial growth temperature of GeSn. This result indicates that crystallization from amorphous GeSn (a-GeSn) may offer better metastability compared to direct epitaxial growth of GeSn. Attesting to the high crystallinity, a peak optical gain of 2,900 cm −1 with a lifetime approaching 0.1 ns is achieved at λ = 2,200-2,350 nm at 300 K. The gain lifetime is on the same order as epitaxial GeSn, and it is >100x longer than the direct gap transition in Ge, confirming the indirect-to-direct band gap transition in GeSn at ∼9 at. Sn composition. Moreover, a prototype p-GeSn/n-Si photodiode from a-GeSn crystallization achieves 100 mA/W responsivity at λ = 2,050 nm and T = 300 K, approaching the level of some commercial PbS detectors. The device also demonstrates photovoltaic behavior and a low dark current density of 1 mA/cm 2 at −1 V reverse bias, comparable to epitaxial Ge/Si photodiodes. These results indicate that crystallization of GeSnOI offers a promising solution for active devices toward 3D MIR photonic integration and/or MIR photonics on flexible substrates.