Although aluminum has a smaller modulus in {111}〈112̄〉 shear than that of copper, we find by first-principles calculation that its ideal shear strength is larger because of a more extended deformation range before softening. This fundamental behavior, along with an abnormally high intrinsic stacking fault energy and a different orientation dependence on pressure hardening, are traced to the directional nature of its bonding. By a comparative analysis of ion relaxations and valence charge redistributions in aluminum and copper, we arrive at contrasting descriptions of bonding characteristics in these two metals that can explain their relative strength and deformation behavior.