The methylation of various aldehydes, such as acetaldehyde, propionaldehyde, and phenylacetaldehyde over titanium oxide-supported vanadium oxide was studied under atmospheric pressure and temperatures of 250-400 degrees C. The catalyst properties of titanium oxide can be enhanced only by addition of a fairly small amount of vanadium. High-temperature treatment transforms titanium oxide, the support, from anatase to rutile, which causes the catalysts to lose their catalytic properties. The reactivity of these can be ranked in the following order : acetaldehyde > propionaldehyde > phenylacetaldehyde. The steric effect of the substituted groups in propionaldehyde or phenylacetaldehyde may prevent self-condensation to form oligomers and to give a high selectivity of alkylated products.