Indium selenide,a Ⅲ-Ⅴ group semiconductor with layered structure,attracts intense attention in various photoelectric applications,due to its outstanding properties.Here,we report super deformability and thermoelectricity of γ-InSe single crystals grown by modified Bridgeman method.The crystal structure of InSe is studied systematically by transmission electron microscopy methods combined with x-ray diffraction and Raman spectroscopy.The predominate phase of γ-InSe with dense stacking faults and local multiphases is directly demonstrated at atomic scale.The bulk γ-InSe crystals demonstrate surprisingly high intrinsic super deformative ability which is highly pliable with bending strains exceeding 12.5％ and 264％ extension by rolling.At the meantime,InSe also possesses graphite-like features which is printable,writable,and erasable.Finally,the thermoelectric properties of γ-InSe bulk single crystals are preliminary studied and thermal conductivity can be further reduced via bending-induced defects.These findings will enrich the knowledge of structural and mechanical properties' flexibility of InSe and shed lights on the intrinsic and unique mechanical properties of InSe polytypes.