Biocompatible biomimetic materials that exhibit desirable mechanical properties while also encouraging cell ingrowth and proliferation are described. The biomaterials include a multi-layer laminate of three or more decellularized aligned collagen tissues. The individual layers are aligned with one another in an angle-ply arrangement, with the collagen of each layer aligned at an angle to the collagen of the adjacent layer. The biomaterials are useful as collagenous graft materials such as a patch for a hernia in an annulus fibrosus or grafting materials for repair of tendons, ligaments, cartilage and other musculoskeletal tissues.