In this study, the SmFe2 alloy in a high-purity single-phase state has been prepared by the induction melting technique. The surface features of the alloy at room temperature were investigated using the atomic-force and magnetic-force microscopy. The forming of heterogeneous granular structure was revealed, the main structural elements were determined. The presence of the complex domain structure was shown, its description was presented and the domain sizes were found. The results of X-ray structural studies over the temperature range from 100 to 300 K were presented. The experimental data on the temperature dependences of magnetostriction in magnetic fields up to 1.2 T were obtained and analyzed in the region of the spin-reorientational phase transition. The existence of the “angular” phase was indirectly confirmed, its temperature boundaries were refined.