Graphene metamaterials with a radial-like structure and negative Poisson’s ratio (NPR) were assembled using a unique centripetal freezing technique. Driven by the centripetal temperature gradient, ice crystals were grown toward the center of an aqueous graphene dispersion and form a radially arranged skeleton. A reentrant structure was formed at the diagonal of the monolith as the ice crystals sublimate. The obtained centripetal graphene metamaterial (CGM) was endowed with NPR response. CGM maintained NPR under 50% compression, which reached a minimum (−0.18) at 10% strain. After 50 compressive cycles at 50% strain, CGM retained approximately 96% of the original compressive strength. The radial channels endowed CGM with fast absorption kinetics, and the NPR response effectively accommodated the damage caused by volume shrinkage during repeated adsorption-regeneration cycles. This strategy is an effective method for achieving NPR response and improving the mechanical properties of porous materials.