Building structures are prone to cracking, leakage, and corrosion under complex loads and harsh marine environments, which seriously affect their durability performance. To design cementitious composites with excellent mechanical and impermeability properties, Engineered Cementitious Composites (ECCs) doped with ultrahigh molecular weight polyethylene short-cut fibers (PE-ECCs) were used as the reference group. Different types (XYPEX-type from Canada, SY1000-type from China) and doses (0%, 0.5%, 1.0%, 1.5%, 2.0%) of Cementitious Capillary Crystalline Waterproofing materials (CCCWs) were incorporated. The effect of CCCWs on the mechanical and impermeability properties of PE-ECCs, and the microscopic changes, were investigated to determine the best type of CCCW to use and the best amount of doping. The results showed that with increasing the CCCW dosage, the effects of both CCCWs on the mechanical and impermeability properties of PE-ECC increased and then decreased, and that the best mechanical and impermeability properties of PE-ECC were achieved when the CCCW dosing was 1.0%. The mechanical properties of the PE-ECC were more obviously improved by XYPEX-type CCCW, with a compressive strength of 53.8 MPa, flexural strength of 11.8 MPa, an ultimate tensile stress of 5.56 MPa, and an ultimate tensile strain of 7.53 MPa, which were 37.95%, 53.25%, 14.17%, and 21.65% higher than those of the reference group, respectively. The effects of the two CCCWs on impermeability were comparable. CCCW-PE-ECC(X1.0%) and CCCW-PE-ECC(S1.0%) showed the smallest permeation heights, 2.6 mm and 2.8 mm, respectively. The chloride ion diffusion coefficients of CCCW-PE-ECC(X1.0%) and CCCW-PE-ECC(S1.0%) exhibited the smallest values, 0.15 × 10-12 m2/s and 0.10 × 10-12 m2/s, respectively. Micromorphological tests showed that the particle size of the XYPEX-type CCCW was finer, and the intensity of the diffraction peaks of C-S-H and CaCO3 of PE-ECC increased after doping with two suitable doping amounts of CCCW. The pore structure was improved, the surface of the matrix was smoother, and the degree of erosion of hydration products on the fiber surface was reduced after chloride ion penetration. XYPEX-type CCCW demonstrated a more obvious improvement in the PE-ECC pore structure.