The strip casting technique was first used in this work to prepare the Sm2Fe17 parent alloys. Next, the Sm2Fe17N3 powders were synthesized using a gas–solid reaction of Sm2Fe17 powders with N2. Then, the anisotropic Sm2Fe17N3 powders with high performance were prepared by a surfactant-assisted grinding method in gasoline solvent. It was found that the coercivity (iHc) of ground powders increases with decreasing the average particle size (Dm), while the saturation magnetization (Ms) decreases. The maximum value of iHc of 17.5 kOe was obtained at the Dm = 1.3 µm. The ground powders with Dm of 3.1 µm show a remanence ratio (Mr/Ms) over 95% and a maximum energy product [(BH)max] of 35 MGOe. The Sm2Fe17N3 powder exhibited a very high iHc of 36.1 kOe at 10 K. Above 300 K, Sm2Fe17N3 powders mixed with epoxy resin showed a low remanence temperature coefficient of α(RT-100°C) = −0.077% °C−1.