Despite considerable effort, the dielectric constant of interfacial water at solid surfaces is still not fully understood, thus hindering our understanding of the ubiquitous physical interactions in many materials and biological surfaces. In this study, we used molecular dynamics simulations to show that the parallel dielectric constant at the solid/water interface depends on solid-water interactions as well as the interfacial water structure on various solid crystal faces. In particular, ordered water structures can lead to a significant reduction (∼44%) in the parallel dielectric constant at the solid/water interface compared with that of bulk water. This sharp decrease in the parallel dielectric constant can be attributed to the specific antiferroelectric ordered structure of interfacial water molecules, which significantly suppresses the amplitude of the dipolar fluctuation associated with both the number of hydrogen bonds and the degree of order of interfacial water.