Cu-containing layered double hydroxides with different Cu : Al ratios are synthesized by co-precipitation using a mixture of hydroxide and sodium carbonate as a precipitation agent. The influence of the precipitation agent concentration on the formation of the hydrotalcite phase was studied by thermal analysis and X-ray diffraction. The surface of the obtained samples after calcination at 450°C and their subsequent reduction at 300°C in hydrogen, was characterized by X-ray photoelectron spectroscopy and transmission electron microscopy. The synthesized catalysts were tested in the reaction of N-methylation of p-anisidine with methanol in an autoclave reactor to produce N-methyl-p-anisidine. The influence of the Cu : Al ratio in them on the catalytic activity and selectivity was studied.