A new series of organic-inorganic hybrid porous gadolinium phosphonate (GdP) materials have been synthesized using benzene-1,3,5-triphosphonic acid as a phosphonic acid linker through a simple hydrothermal technique. The particle size and morphology are well controlled through the selection of suitable reaction conditions. The obtained materials exhibit very high specific surface area and crystalline pore walls with a triclinic structure having unit cell parameters a = 7.76 (3) A; b = 8.60 (6) A; c = 14.09 (7) A; [small alpha] = 100.08 (4)[degree]; [small beta] = 84.23 (6)[degree]; [gamma] = 116.29 (6)[degree]. The obtained GdP materials are further used as a magnetic resonance imaging (MRI) contrast agent with r1 and r2 values of 2.6 and 4.7 s-1 mM-1, respectively.