A new layered zinc phosphate (Mu-39) has been synthesized by hydrothermal treatment with biomolecules as original templates. It was synthesized with the L-histidine amino acid (C 6 H 9 N 3 O 2 ). The structure was determined by a single crystal X-ray diffraction study combined with exhaustive solid-state NMR experiments. These last ones [ 1 H f 13 C HETCOR, 1 H single quantum/double quantum (DQ), 31 P, 1 H f 31 P CPMAS, 1 H f 31 P HETCOR] ascertained the formulation of Mu-39 as {[C 6 H 10 N 3 O 2 þ ][Zn 2 (HPO 4 )(PO 4 ) -] 3 H 2 O} n with a hydrogen phosphate and phosphate ligands, and ruled out partial protonation such as (H 1-x PO 4 )(H x PO 4 ). A 31 P magic angle spinning (MAS) NMR study supported the almost complete racemization of L-histidine during the hydrothermal synthesis with only a small enantiomeric excess of 25% remaining. The compound crystallizes in the triclinic symmetry (space group P1) with a = 8.6109(6) Å , b = 9.0319(6) Å , c = 9.9523(7) Å , and R = 84.481(2)°, β = 83.279(2)°, γ = 74.652(2)°, V = 739.56(9) Å 3 , Z = 2. The inorganic layer is built up from four-membered rings sharing T-O-T bonds (T = Zn and P) and connected to each other in order to form ladders which are joined together via a Zn-O-P bond for creating eight-membered rings. The interest and the originality of this new zinc phosphate come especially from its unusual stability in aqueous solution.