Articular cartilage plays an important role in synovial joint function, but this function is diminished when cartilage tissue breaks down in osteoarthritis. Tissue engineering is a promising approach for replacing failed cartilage, as cartilage is a relatively simple tissue with no blood supply and very few biological cells. To imitate the structure of natural cartilage extracellular matrix material, three components must be included: the hydrated ground substance, the charges that contribute to compressive stiffness via electrostatic repulsion, and the nanofibrous collagen network that resists tensile deformation and failure. Here, the nanofiber network is considered, with examination of its fracture behavior in an as-electrospun state and following a mild chemical crosslinking process. Mode III fracture testing was used to quantify the tear toughness of the fibrous mats, and failure behavior was qualitatively examined with scanning electron microscopy. In ongoing work, this nanofibrous structure will be combined with a charged polyelectrolyte hydrogel gel to create a biomimetic cartilage-like material. By using biomimicry to replicate what is present in native cartilage tissue, a superior material can be designed and fabricated for use in tissue repair and replacement.