Bimetallic Fe-Mn oxide (BFMO) has been regarded as a promising activator of peroxysulfate (PS), the sustained activity and durability of BFMO for long-term activation of PS in situ, however, is unclear for groundwater remediation. A BFMO (i.e., Mn1.5FeO6.35) was prepared and explored for PS-based in situ chemical oxidation (ISCO) of trichloroethylene (TCE) in sand columns with simulated/actual groundwater (SGW/AGW). The sustained activity of BFMO, oxidant utilization efficiency, and postreaction characterization were particularly investigated. Electron spin resonance (ESR) and radical scavenging tests implied that sulfate radicals (SO4•-) and hydroxyl radicals (HO•) played major roles in degrading TCE, whereas singlet oxygen (1O2) contributed less to TCE degradation by BFMO-activated Oxone. Fast degradation and almost complete dechlorination of TCE in AGW were obtained, with reaction stoichiometry efficiencies (RSE) of ΔTCE/ΔOxone at 3-5%, much higher than those reported RSE values in H2O2-based ISCO (≤0.28%). HCO3- did not show detrimental effect on TCE degradation, and effects of natural organic matters (NOM) were negligible at high Oxone dosage. Postreaction characterizations displayed that the BFMO was remarkably stable with sustained activity for Oxone activation after 115 days of continuous-flow test, which therefore can be promising catalyst for Oxone-based ISCO for TCE-contaminated groundwater remediation.