A zero-valent iron pillared montmorillonite repair material relates to the field of environmental functional materials. A preparation method thereof is mainly to obtain the zero-valent iron pillared montmorillonite repair material by reducing hydroxyl-iron pillared montmorillonite at high temperature in a mixed atmosphere of hydrogen and nitrogen, and mainly includes: (1) preparation of Na-montmorillonite; (2) preparation of a polyhydroxy-iron pillared solution; (3) preparation of hydroxy-iron pillared montmorillonite; and (4) obtaining the zero-valent iron pillared montmorillonite repair material by means of high-temperature reduction-calcination in the mixed atmosphere of hydrogen and nitrogen. The zero-valent iron pillared montmorillonite repair material can be used for removing degradation-resistant organic pollutants, and degrading organics into small molecular organics by means of peroxymonosulfate (PMS).