The development of strategic methods to enhance the catalytic reactivity and electron efficiency of biocharmodified zero-valent iron (BC-ZVI) via mechanochemistry is highly important and desirable for the use of peroxydisulfate-based advanced oxidation processes (PDS-AOPs) in soil remediation. Herein, novel amphiphilic ball-milled N-doped biochar-ZVI composites (NBC-ZVIbm) were fabricated to activate PDS for efficient pyrene degradation in soil. The N-doped site- and alloying heterojunction-induced surface charge redistribution, directional electron transfer, and amphiphilicity of NBC-ZVIbm were verified, all of which improved the interactions among NBC-ZVIbm, PDS and pyrene. Specifically, NBC incorporation optimized PDS oxidation and pyrene adsorption on NBC-ZVIbm, forming a reaction center that efficiently accelerated the reaction. As a result, 95.5 % of 98.3 mg/kg pyrene in soil was degraded by NBC-ZVIbm/PDS within 7 d, which was 2.3 and 1.5 times greater than that of ball-milled ZVI and BC-ZVIbm, respectively; additionally, the electron efficiency of this process increased to 85.2 %. Characterization of the reaction process suggested that NBC incorporation induced directional electron transfer from ZVI to NBC for PDS activation and SO4 center dot- generation. Subsequently, the amphiphilicity of NBC-ZVIbm promoted soil phase-pyrene desorption and migration, thereby increasing pyrene degradation. This NBC-incorporation method provides a strategy for constructing highly efficient ZVI-based catalysts for the use of PDS-AOPs in soil remediation.