The ultrathin SmCo5 nanoflakes with average thickness smaller than 50 nm are prepared by a novel method of solid particle (NaCl) and surfactant co-assisted ball milling. The as-prepared nanoflakes exhibit a narrower thickness distribution of 10-50 nm and high coercivity of 23 kOe. The possible formation mechanism of nanoflakes are proposed. Temperature dependence of demagnetization curves indicate that the magnetization reversal may be controlled by both nucleation and pinning. The results of X-ray powder diffraction and magnetic measurement for aligned SmCo5 nanoflakes resin composite indicate that the nanoflakes have a high texture degree. The ultrathin thickness and high coercivity are beneficial for preparing the high performance soft/hard coupling magnets and nanocomposite magnets.