The dependence of electric quadrupole splitting of nuclear magnetic resonance absorption lines in single crystals on crystal orientation in an external magnetic field is investigated theoretically following earlier work of Pound, of Volkoff, Petch, and Smellie, and of Bersohn. Explicit formulae are given, applicable to non axially symmetric crystalline electric field gradients (η ≠ 0), and valid up to terms of the second order in the quadrupole coupling constant , for the dependence of the absorption frequencies on the angle of rotation of the crystal about any arbitrary axis perpendicular to the magnetic field. Some formulae including third order effects in Cz are also given. It is shown that an experimental study of the dependence of this splitting on the angles of rotation about any two arbitrary mutually perpendicular axes is sufficient, when second order effects are measurable, to yield the values of | Cz |, η, and the orientation of the principal axes of the electric field gradient tensor at the nuclear sites. In the case that the direction of one of the principal axes is known from crystal symmetry, a single rotation about this axis gives the complete information.A new method of determining nuclear spin I is proposed which depends on comparing first and second order shifts of the resonance frequencies of the strong inner line components. The method will be of interest in those cases where the total number 2I of line components can not be unambiguously ascertained owing to the outer line components being excessively broadened and weakened by crystal imperfections.