Defects in the interfacial transition zone (ITZ) between recycled tire rubber and cement matrix obstacle to the large-scale application of sustainable rubberized cementitious materials. This paper proposed and evaluated different targeted treatment methods for micro-surface properties enhancement of rubber aggregate by the Polyvinyl Alcohol (PVA), Polyethylene Glycol-200 (PEG), and Hydroxypropyl methylcellulose (HY) polymer solutions through copolymerization and drafting processes. The optimum modification condition was determined through the FT-IR analysis, contact angle, and surface free energy of treated rubber aggregates and the micro-surface morphology and element distribution were analyzed by using ESEM and EDX, respectively. The flexural strength and pore size distribution of steel fiber-reinforced rubberized mortar with relatively high replacing volumes (20%, 40%, and 60%) were evaluated to validate the targeted micro-surface modification efficiency. The surface microstructure and hydrophilic properties of rubber aggregate were significantly improved and the mechanism for enhancing the interface adhesion between rubber and cement matrix was revealed.