Italy’s architectural heritage, particularly masonry vaults, is highly susceptible to seismic damage, presenting significant preservation challenges. In addition to the more widely known reinforcement techniques, such as Fibre-Reinforced Polymers (FRP) and Fibre-Reinforced Cementitious Matrixes (FRCMs), there has been a growing interest in sustainable and eco-friendly solutions. A notable example of this is a composite material that integrates mono- or bi-directional hemp ropes into a traditional cocciopesto matrix. To further assess this material, unreinforced and strengthened at the extrados using the hemp-based composite full-scale masonry vaults were built. These specimens were subjected to an increasing level of seismic load on the 6-DOF shaking table at the L.E.D.A. Research Institute of the Kore University of Enna, Italy. A motion capture system, by means of high-resolution cameras and reflective markers, was used to monitor the vaults’ behavior during testing. This system captured detailed displacement time histories and spatial components, allowing for comprehensive data analysis. To monitor the progressive formation of structural hinges under increasing seismic intensity, the vaults were equipped with a dense network of reflective markers. This enabled for precise tracking of hinge openings and damage evolution in both unreinforced and reinforced specimens. This study highlights the efficacy of displacement tracking and bio-composite strengthening in mitigating seismic vulnerabilities, providing valuable insights into sustainable strategies for preserving historic masonry structures.