Nanoscale defects such as dislocations have a profound impact on the physics of crystalline materials. Understanding and characterizing the motion of screw dislocation and its corresponding effects on the mechanical properties of complex low-symmetry materials has long been a challenge. Herein, we focus on triclinic tobermorite, as a model system and a crystalline analogue of layered hydrated cement, and report for the first time how the motion of screw dislocation can influence the strengthening–toughening relationship, imparting brittle-to-ductile transitions. By applying shear loading in tobermorite systems with single and dipole screw dislocations, we observe dislocation jogs around the dislocation core, which increases the yield shear stress and the work-of-fracture when the dislocation lines are along the [100] and [010] directions. Our results demonstrate that the dislocation core acts as a bottleneck for the initial straight gliding to induce intralaminar gliding, which consequently leads to a significant improvement in the mechanical properties. Together, the fundamental knowledge gained in this work on the role of the motion of the dislocation core on the mechanical properties provides an improved understanding of deformation mechanisms in cementitious materials and other complex layered systems, providing new hypotheses and design guidelines for the development of strong, ductile, and tough materials.