Zn(CN)2 is an important material because it shows isotropic NTE over a large temperature range and to an extent more than double that of ZrW2O8. This unusual behaviour originates from its extreme strucutral flexibility, which is itself a property of the underconstrained Zn-CN-Zn linkages from which the structure is assembled. One might expect this same flexibility to produce unusual behaviour under pressure, and indeed some recent data collected on PEARL during instrument commissioning suggest the material undergoes reversible pressure-induced amorphisation at a pressure of ~3 GPa. Our aim in this study is to expand on this preliminary investigation and to obtain detailed structural information concerning the high-pressure behaviour of Zn(CN)2, exploiting the sensitivity of neutrons to the positions of C/N atoms to identify its mechanism of compression and the implications for NTE.