Activated carbons have been prepared by the chemical activation of olive stones with phosphoric acid and loaded with Zr. The addition of Zr to the phosphorus-containing activated carbons resulted in the formation of zirconium phosphate surface groups. Gas phase methanol dehydration has been studied while using the prepared Zr-loaded P-containing activated carbons as catalysts. Carbon catalysts showed high steady-state methanol conversion values, which increased with Zr loading up to a limit that was related to P content. The selectivity towards dimethyl ether was higher than 95% for all Zr loadings. Zirconium phosphate species that were present on catalysts surface were responsible for the catalytic activity.