The elastic and structural behaviour of the synthetic zeolite CsAlSi 5 O 12 (a = 16.753(4), b = 13.797(3) and c = 5.0235(17) A ˚, space group Ama2, Z = 2) were investigated up to 8.5 GPa by in situ single-crystal X-ray diffraction with a diamond anvil cell under hydrostatic conditions. No phase-transition occurs within the P-range investigated. Fitting the volume data with a third-order Birch-Murnaghan equation-of-state gives: V 0 = 1,155(4) A ˚3, K T0 = 20(1) GPa and K 0 = 6.5(7). The ''axial moduli'' were calculated with a third-order ''linearized'' BM-EoS, substituting the cube of the individual lattice parameter (a 3 , b 3 , c 3 ) for the volume. The refined axial-EoS parameters are: a 0 = 16.701(44) A ˚, K T0a = 14(2) GPa (b a = 0.024(3) GPa -1 ), K 0 a = 6.2(8) for the a-axis; b 0 = 13.778(20) A ˚, K T0b = 21(3) GPa (b b = 0.016(2) GPa -1 ), K 0 b = 10(2) for the b-axis; c 0 = 5.018(7) A ˚, K T0c = 33(3) GPa (b c = 0.010(1) GPa -1 ), K 0 c = 3.2(8) for the c-axis (K T0a :K T0b :K T0c = 1:1.50:2.36). The HP-crystal structure evolution was studied on the basis of several structural refinements at different pressures: 0.0001 GPa (with crystal in DAC without any pressure medium), 1.58(3), 1.75(4), 1.94(6), 3.25(4), 4.69(5), 7.36(6), 8.45(5) and 0.0001 GPa (after decompression). The main deformation mechanisms at high-pressure are basically driven by tetrahedral tilting, the tetrahedra behaving as rigid-units. A change in the compressional mechanisms was observed at P B 2 GPa. The P-induced structural rearrangement up to 8.5 GPa is completely reversible. The high thermo-elastic stability of CsAlSi 5 O 12, the immobility of Cs at HT/HP-conditions, the preservation of crystallinity at least up to 8.5 GPa and 1,000°C in elastic regime and the extremely low leaching rate of Cs from CsAlSi 5 O 12 allow to consider this openframework silicate as functional material potentially usable for fixation and deposition of Cs radioisotopes.