The preparation of N-methylaniline in two various processes: alkylation of aniline with methanol and hydroalkylation of nitrobenzene with methanol has been studied. Bifunctional molecular sieves containing metal copper as the hydrogenating component and zeolites BEA, MOR, MFI, FAU (Y) and mesoporous material MCM-41 as an alkylating component were used as catalysts. It has been shown that the modification of samples with copper nitrate increases the number of Lewis acid sites and decreases the number of Bronsted acid sites as copper embeds into cation exchange positions. It has been determined that the catalyst modification with copper increases the activity and enhances the selectivity towards N-alkylated products.