A shear-punch test (SPT) experimental method was developed to address the lack of shear deformation and failure response data for the human skull as a function of local bone microarchitecture. Improved understanding of skull deformation and fracture under varying stress-states helps implement mechanism-based, multi-axial material models for finite element analysis for optimizing protection strategies. Shear-punch coupons (N = 47 specimens) were extracted from right-parietal and frontal bones of three fresh-frozen-thawed human skulls. The specimens were kept as full through-thickness or segmented into the three skull constituent layers:​ the inner and outer cortical tables and the middle porous diploë. Micro-computed x-ray tomography (μCT) before and after SPT provided the bone volume fraction (BVF) as a function of depth for correlation to shear mechanisms in the punched volumes. Digital image correlation was used to track displacement of the punch above the upper die to minimize compliance error. Five full-thickness specimens were subjected to partial indentation loading to investigate the process of damage development as a function of BVF and depth. It was determined that BVF dominates the shear yield and ultimate strength of human skull bone, but the imposed uniaxial loading rate (0.001 and 0.1 s⁻¹) did not have as strong a contribution (p = 0.181–0.806 > 0.05) for the shear yield and ultimate strength of the skull bone layer specimens. Shear yield and ultimate strength data were highly correlated to power law relationships of BVF (R² = 0.917–0.949). Full-thickness and partial loaded SPT experiments indicate the diploë primarily dictates the shear strength of the intact structure.