Keratin is one of the most common structural biopolymers exhibiting high strength, toughness, and low density. It is found in various tissues such as hairs, feathers, horns, and hooves with various functionalities. For instance, horn keratin absorbs a large amount of energy during intraspecific fights. Keratinized tissues are permanent tissues because of their basic composition consisting of dead keratinized cells that are not able to remodel or regrow once broken or damaged. The lack of a self-healing mechanism presents a problem for horns as they are under continued high risk from mechanical damage. In the present work, we show for the first time that a combination of material architecture and a water-assisted recovery mechanism, in the horn of bighorn sheep, endows them with shape and mechanical property recoverability after being subjected to severe compressive loading. Moreover, we unravel the effect of hydration, on the material molecular structure and mechanical behavior, by means of synchrotron wide angle X-ray diffraction, Fourier transform infrared spectroscopy, nanoindentation, and in-situ and ex-situ tensile tests. The recovery and remodeling mechanism is anisotropic and quite distinct to the self-healing of living tissue such as bones.