In article number 2109304, Glaucio H. Paulino and co-workers report spinodal architected materials with tunable anisotropy to unify optimal design and manufacturing of multiscale structures. Mechanical anisotropy and porosity are spatially tailored to directly target mechanical function (e.g., stiffness) and indirectly promote biological function (e.g., fluid transport conduits). Applications to medical (e.g., prosthetics) and mechanical components are demonstrated.