- We report on an experimental and theoretical nuclear quadrupole resonance (NQR) multiple-pulse spin-locking study of the thermal mixing process in solids containing nuclei of two different sorts, I>1/2 and S = 1/2, coupled by dipole–dipole interactions and influenced by an external magnetic field. Two coupled equations for the inverse spin temperatures of both the spin systems describing the mutual spin–lattice relaxation and the thermal mixing were obtained using the method of the nonequilibrium state operator. It is shown that the relaxation process is realized with non-exponential time dependence described by a sum of two exponents. The calculated relaxation time versus the multiple-pulse field parameters agrees well with the obtained experimental data in 1,4-dichloro-2-nitrobenzene. The calculated magnetization relaxation time versus the strength of the applied magnetic field agrees well with the obtained experimental data.