AbstractNatural fractures in shale and sandstone that formed under diagenetic and metamorphic conditions are frequently filled with mineral cement that lack residual fracture porosity visible under the petrographic microscope and that are generally interpreted to be impermeable. Scanning electron microscopy of calcite, dolomite, quartz, and barite fracture cement from low‐permeability, diagenetically altered shale and sandstone formations provides evidence of open and variably connected elongate pores or gaps with apertures of 10–600 nm, referred to as nanoscale grain boundary channels (NGBC). Electron backscatter diffraction of samples prepared using broad ion‐beam milling shows that NGBCs occur along grain boundaries of blocky or columnar fracture cement. Grain boundaries are either faceted or display undulation at the nanometer scale. NGBCs tend to increase in aperture with increasing maximum formation burial temperature, indicating dissolution‐precipitation kinetics influences grain boundary structure. Transmission electron microscopy reveals heterogeneous crystallographic domains with possible amorphous regions bridging across grain boundary channels. We propose a model of dynamic concurrent dissolution‐precipitation along grain boundaries that preserves NGBCs in carbonate and quartz fracture cements that have experienced diagenetic to low‐grade metamorphic conditions. While partially healed, NGBCs may be sufficiently connected to increase permeability of low‐permeability formations containing cemented fractures.