Multilayered composites (MLCs) processed using accumulative roll bonding (ARB) have great potential as candidates for perforation testing. In the current study, multilayered composites comprised of alternating layers of titanium and aluminum have been investigated. Since the ARB process has been shown to induce anisotropy, the Ti/Al MLCs were first subjected to quasi-static loading to determine the effects of anisotropy. The MLCs were then subjected to perforation testing using projectiles with various apex angles. The effects of perforation testing were studied in terms of varying ballistic parameters and characterization of the fracture surfaces of the MLCs. The results of this study show that ARB-processed Ti/Al MLCs are promising for use in ballistic and impact applications.