The layered structure of tetragonal Ni(CN)2, consisting of square-planar Ni(CN)4 units linked in the a-b plane, with no true periodicity along the c-axis, is expected to show anisotropic compression on the application of pressure. High-pressure neutron diffraction (elastic) and inelastic neutron scattering experiments have been performed on polycrystalline Ni(CN)2 to investigate its compressibility and stability. The intralayer a lattice parameter does not show any appreciable variation with increase of pressure up to 2.7 kbar. Above this pressure value, a decrease in a is observed. The c lattice parameter decreases slowly up to 1 kbar, then decreases sharply up to 20 kbar. It does not show any significant variation with further pressure increase up to 50 kbar. The response of the lattice parameters to the applied pressure is strongly anisotropic as the interlayer spacing (along the c-axis) shows a significantly larger contraction than the a-b plane. The experimental pressure dependence of the volume data is fitted to a bulk modulus, B0, of 1050 (20) kbar over the pressure range 0-1 kbar, and to 154 (2) kbar in the range 1-50 kbar. The change in the slope of the lattice parameters at 1 kbar is also supported by high-pressure Raman measurements, which indicate a phase transition at 1 kbar. Probably arising from a change in the CN ordering within the Ni(CN)2 layers. Raman measurements, performed up to 200 kbar, highlight the possible existence of a second phase transition taking place at about 70 kbar. Our neutron inelastic scattering measurements of the pressure dependence of the phonon spectra performed up to 2.7 kbar, also support the occurrence of a phase transition at low pressure.