Superior soft-magnetic materials are necessary for the development of modern magnetic devices with energy-saving and high-power density requirements. However, improving the magnetism by nanocrystallization always brings about the sacrifice of resistivity, presenting a common trade-off in Fe-based amorphous-nanocrystalline alloys. Here, the comprehensive merits of both superior soft-magnetic properties (high saturation magnetization of 1.81 T and low coercivity of 3.8 A/m) and high resistivity of 117.2 μΩ·cm were obtained by precisely tailoring amorphous-nanocrystalline microstructure close to electrical percolation threshold for a Fe82.5B12P2C1Cu0.5Co2 amorphous alloy. The soft-magnetic properties are attributed to the low magnetic anisotropy stemming from high nuclei number density and ultrafine nanocrystalline grains of 9.2 nm. The high resistivity is associated with the electrical percolation behavior with a nanocrystalline volume threshold of 14.8 % in the composite alloy. The results provide an effective strategy to overcome the trade-off in traditional amorphous-nanocrystalline alloys, significant for applications in high-frequency, high-power, and energy-saving devices.