Nano-particles and fibers-modified cementitious composite (NFCC) can greatly overcome the shortcomings of traditional cementitious materials, such as high brittleness and low toughness, and improve the durability of the composite, which in turn increases the service life of the structures. Additionally, the polymer coatings covering the surface of the composite can exert a good physical shielding effect on the external water, ions, and gases, so as to improve the permeability and chloride ion penetration resistance of the composite. In this study, the effect of three types of polymer coatings on the water contact angle, permeability resistance, and chloride ion penetration resistance of the NFCC with varied water–binder ratios were investigated. Three kinds of polymers (chlorinated rubber coating, polyurethane coating, and silane coating) were applied in two types of coatings, including single-layer and double-layer coatings. Three water–binder ratios of 35 wt.%, 40 wt.%, and 45 wt.% were used for the NFCC. The research results revealed that the surface of the NFCC treated with polymer coatings exhibited excellent hydrophobicity. The permeability height and chloride diffusion coefficient of the NFCC coated with different types of polymer coatings were 31–48% and 36–47% lower, respectively, than those of the NFCC without polymer coatings. The durability of the NFCC was further improved when the polymer coatings were applied to the surface in two-layer. Furthermore, it was discovered that increasing the water–binder ratio of the NFCC would lessen the positive impact of polymer coatings on the durability of NFCC.