For the characteristic that the mechanical properties of resin composite are lower than cast iron, steel fibers are used to improve its properties in this paper. A weak interfacial bonding strength between steel fibers and resin indicates that steel fibers’ property cannot perform well in the polymer. In order to improve the interfacial bonding strength, four methods of surface treatment, phosphating, acid pickling, oxidation, and coupling are applied to steel fibers, and the corresponding pull-off tests are carried out to compare with untreated steel fibers. Research results show that the maximum interfacial bonding strength is increased by 45.1% after coupling treatment.