Novel α-alumina crystalline nanosheets are used for the preparation of alumina-carbon composites, in which the latter component is phenolic resin-based ordered mesoporous carbon. A unique feature of these composites is perpendicular orientation of ordered mesopores of the carbon to the (001) facets of nonporous α-alumina nanosheets accompanied by significant enlargement of these mesopores in comparison to those present in the bulk carbon.