Buckyrock is a three-dimensional, solid block material comprising an entangled network of single-wall carbon nanotubes (SWNT), wherein the block comprises greater than 75 wt % SWNT. SWNT buckyrock is mechanically strong, tough and impact resistant. The single-wall carbon nanotubes in buckyrock form are present in a random network of individual single-wall carbon nanotubes, SWNT “ropes” and combinations thereof. The random network of the SWNT or SWNT ropes can be held in place by non-covalent “cross-links” between the nanotubes at nanotube contact points. In one embodiment, SWNT buckyrock is made by forming a SWNT-water slurry, slowly removing water from the slurry which results in a SWNT-water paste, and allowing the paste to dry very slowly, such that the SWNT network of the SWNT-water paste is preserved during solvent evaporation. Buckyrock can be used in applications, such as ballistic protection systems, involving light-weight material with mechanical strength, toughness and impact resistance.