The crystal structure of LiNO3 is determined by single-crystal X-ray diffraction. The structure is isomorphous with that of calcite; lithium is coordinated by oxygen in a trigonally-elongated octahedron. A positive sign of the Li-7 quadrupole coupling constant is deduced from a simple point charge model with the following assumptions : (1) only contributions from the six oxygen atoms of the inner coordination sphere are included, and (2) the charge assigned to each oxygen atom is negative. This result is compared to the low-temperature Li-7 NMR work of Kuhns and Waugh (J. Chem. Phys. 1992, 97, 2166-2167), in which the sign of the Li-7 quadrupole coupling constant was found to be positive.