Sea urchin spines are an example of a hard natural composite with mineral and organic phases. The role of the organic phase in the response to mechanical stress was assessed by promoting the degradation of such spines by exposing them to ageing and ultraviolet (UV) irradiation. Thermal and structural characterization of the irradiated samples show that this UV irradiation treatment promotes degradation of the organic and inorganic phase of spines. Uniaxial compression tests carried out on aged and UV irradiated samples showed that both treatments affected the mechanical properties of the spines. Scanning electron microscopy (SEM) images of failed specimens were used to analyze the failure mechanisms of the compressed spines. The analysis of the fracture surfaces showed that the failure mechanisms of spines were modified as a consequence of UV irradiation, leading in the last case to mostly brittle fracture surfaces. We suggest that the proteins responsible for the formation of calcite also determine the mechanical properties and the failure mode of spines. This system can be used as a model for the study of the failure modes of other natural and synthetic hard composites.