The consumption of polypropylene (PP) has significantly increased over that of other materials because of its light weight, easy molding, and high mechanical strength. However, the applications of PP are limited, owing to the lack of surface properties, especially with respect to adhesive properties and hydrophilicity. In this study, we developed a surface modification method for enhancing the adhesive properties and hydrophilicity on the PP surface using a side-chain crystalline block copolymer (SCCBC). This method was simple and involved the dipping of a PP film in a diluted SCCBC solution. The optimized modification conditions for enhancing the adhesive properties of PP were investigated. The results revealed that the adhesion strength of PP modified with the SCCBC of behenyl acrylate and 2-(tert-butylamino)ethyl methacrylate was enhanced to 2.00 N/mm (T-peel test) and 1.05 N/mm2 (tensile shear test). In addition, the hydrophilicity of PP modified with the SCCBC of behenyl acrylate and di(ethylene glycol)ethyl ether acrylate was enhanced to a water contact angle of 69 ± 4°. Surface analysis was also performed to elucidate a plausible mechanism for PP modification by the SCCBCs. This surface modification method is facile and enhances desirable properties for the wide application of PP.