Fe-based amorphous powder cores (AMPCs) were prepared from FeSiBCr amorphous powders with phosphate–resin hybrid coating. The high-frequency magnetic properties of AMPCs annealed at different temperatures were systematically studied. After annealing at low temperatures, the effective permeability and core loss improved due to the internal stress of the powder cores being released. The sample annealed at 480 °C exhibits the lowest hysteresis loss of about 29.6 mW/cm³ at 800 kHz as well as a maximum effective permeability of 36.4, remaining stable until 3 MHz, which could be useful for high-frequency applications.