The inorganic-organic hybrid magnesium aminoethyl phosphonate (Mg(AEP)(H(2)O), particle diameter: 20 nm; specific surface area: 322(10) m(2) g(-1); pore volume: 0.9(1) cm(3) g(-1)) shows reversible CO(2) sorption (152(5) mg g(-1)) at high pressure (≤110 bar). In contrast, N(2) uptake remains below 1.0(1) mg g(-1). Based on this selectivity (∼100%) Mg(AEP)(H(2)O) expands the range of materials available for CO(2) capture.