ZnFe2-xAlxO4 (x = 0, 1, 2) spinels were obtained by microwave-assisted solvothermal method using 1,4-butanediol as reaction medium. The results of XRD and HRTEM studies have indicated higher nano-crystallinity of aluminium containing spinels, and N-2 adsorption-desorption measurements have revealed their enhanced textural properties, in particular much higher specific surface areas. NH3-TPD method and cyclohexanol test have shown the variation of surface acid-base properties with the changes in the spinel composition. All studied spinels were active in aniline methylation and proved to be selective for N-methylation leading to N-methylaniline and N,N-dimethylaniline. The main advantage of aluminium containing spinels is that N-alkylation with methanol is possible at significantly lower temperature (200-260 degrees C) when pure zinc ferrite is almost inactive.