Nanomaterials demonstrate novel mechanical properties attributed to the extremely large interfacial area. At quasi-static rates, the interfacial interactions are crucial in mechanical behaviors, however, materials under extreme mechanical stimuli are rarely studied at nanoscale. With an advanced laser-induced projectile impact test, we perform supersonic impact of micro-projectiles on polymer films, multilayer graphene, carbon- based nanocomposites membranes as well as individual micro-fibers, to study the interface interactions in the high-rate regime, and develop a simplified model to characterize the ballistic performance of materials.