Nuclear magnetic resonance (NMR) experiments recording the recovery of the magnetization of the nuclei in one phase, fo[lowing the excitation of the nuclei in the other phase, is a cIassical way of studying blends inhomogeneous at the nanometer scale. Interpretation of the time recovery in terms of the spatial dimension requires knowledge of the two-phase spin diffusion coefficients D o. A new method of measurement of D O is proposed on the basis of variable angle-tilted rotatory frame relaxation in homogeneous samples doped with paramagnetic centers. The choice of the tilt angle allows one to finely balance the direct relaxation by the paramagnetic center and the spin diffusion. The shape of the relaxation is analyzed with the solution for the diffusion-limited regime M(t)/M(O) = exp[-(r2t) la -rlt ] and D O then calculated from rl, r 2 and the concentration of paramagnetic centers. Conditions where reliable results can be obtained both theoretically and numerically ate explored. The method has been implemented and applied to polycrystalline Mn-doped CaF 2 leading to D O = 540+60 nmVs, in agreement with existing values on this model compound.