The large strain mechanical properties of adult porcine gray and white matter brain tissues were measured in shear and confirmed in compression. Consistent with local neuroarchitecture, gray matter showed the least amount of anisotropy, and corpus callosum exhibited the greatest degree of anisotropy. Mean regional properties were significantly distinct, demonstrating that brain tissue is inhomogeneous. Fresh adult human brain tissue properties were slightly stiffer than adult porcine properties but considerably less stiff than the human autopsy data in the literature. Mixed porcine gray/white matter samples were obtained from animals at “infant” and “toddler” stages of neurological development, and shear properties compared to those in the adult. Only the infant properties were significantly different (stiffer) from the adult.