Disclosed herein are improved thermoplastic polyurethane compositions, articles, and related methods. These compositions include aliphatic thermoplastic polyurethanes having a hard segment content ranging from 57 percent to 80 percent by weight. The hard coat compositions have a Shore D hardness of at least 70 and can display an Elongation at Break test result at 25 degrees Celsius of at least 150 percent. These materials, when hardened, can serve decorative and/or protective functions while displaying both a high degree of elongation at moderate temperatures and high hardness.