The spin–lattice relaxation rate of paramagnetic Fe 3+ in single-crystalline ZnO has been determined following low-fluence (Φ< 10 12 cm− 2) 60 keV implantation of 57 Mn+(T 1/2= 1.5 min) and emission Mössbauer spectroscopy on the 57 Fe daughter nucleus in the temperature range from 300 to 664 K. The spin–lattice relaxation of Fe 3+ is found to follow a T 9 temperature dependence, in contrast to the T 2 dependence expected for a two-phonon Raman process determined in both single-crystal MgO and α-Al 2 O 3 using the same analysis method of the Mössbauer spectra measured without an applied external magnetic field. This is an unexpected result since ZnO has a lower Debye temperature than both MgO and α-Al 2 O 3.