The electrical resistivity of hardened cement-based materials was measured in this work by a modified noncontact electrical resistivity measurement (MN-CM). The resistivity was further processed to compute the chloride diffusion coefficient (D ) using the Nernst-Einstein equation. Also, the rapid chloride migration test (RCM) was carried out to obtain the chloride migration coefficient (D ), and the relationship between D and D has been established. The obtained D was further correlated to the pore structure parameters characterized by low-field nuclear magnetic resonance (NMR) spectroscopy. The results show that the D is more sensitive to the change of pore connectivity, while D is more sensitive to the change of porosity. The D is smaller than D since it strictly follows the Nernst-Einstein equation while RCM neglects the other driving forces such as capillary sorption and concentration gradient. It is concluded that the proposed MN-CM can obtain the chloride diffusion coefficient of saturated cement-based materials in a quick, stable, and reliable manner.