Simple molecular solids become unstable at high pressures, typically transforming to dense framework and/or metallic structures. We report formation of an unusual ionic solid NO(+)NO(3)(-) (nitrosonium nitrate) from N(2)O at pressures above 20 GPa and temperatures above 1000 K. Synchrotron x-ray diffraction indicates that the compound crystallizes with a structure related to the aragonite form of CaCO(3) and NaNO(3). Raman and infrared spectroscopic data indicate that the structure is noncentrosymmetric and exhibits a strong pressure dependent charge transfer and orientational order.