A catalytic phenol methylation study on two ferrospinel materials (Mg 0.63 Zn 0.37 )(Mn 0.1 Fe 1.8 )O 3.85 (hereafter Mg− Zn) and (Mn 0.55 Zn 0.35 Fe 0.1 )Fe 2 O 4 (hereafter Mn−Zn) was performed. The reaction was carried out in the gas phase in a continuous manner with the feed composition of phenol, methanol, and water in molar ratio 1:5:1. Both ferrites are active in the studied reaction. The alkylation of phenol with methanol led to the selective production of o-methylated phenol derivatives, i.e., o-cresol and 2,6-xylenol. However, both catalysts markedly differ in terms of activity. Different synergy effects on both catalysts cannot be a sufficient explanation. These materials do not differ significantly either in their susceptibility to reduction or in their Lewis type acidity. Because their microstructure differs significantly, a size effect may therefore be responsible for the differences in activity.