The gas phase dehydration of hexan-1-ol, hexan-2-ol and cyclohexanol (473 K less than or equal to T less than or equal to 573 K) has been studied over NaY, HY and Ni/NaY zeolites and the action of each has been compared with a commercially available 13% w/w Nafion/SiO2 composite, The Ni exchanged zeolite and Nafion catalysts exhibited a high selectivity in terms of all;ene formation. Condensation to generate the respective ether represented a secondary process that was not promoted to the same extent. Reaction over the Nafion sample was characterised by an initial increase in conversion with time that can be linked to a gradual swelling of the polymeric matrix by water produced in the dehydration step. Reduction of the Ni/NaY zeolites in flowing hydrogen generated surface Bronsted acidity that has been characterised by IR, NH3 chemisorption and iodometric titration. Dehydration activity in the case of NaY and Ni/NaY was directly proportional to acid site concentration and there was little dependence on acid site strength. The effect of reaction time, temperature and gas space velocity on activity/selectivity is presented and discussed. Catalysis over the zeolites was accompanied by appreciable deactivation due to coke formation that was also dependent on surface acid site concentration. A high carbon (up to 50% w/w) content was recorded for the spent zeolites but the presence of nickel metal served to limit the deposition of highly amorphous carbonaceous species. The applicability of a reductive regeneration of the used zeolites is considered, Carbon monoxide chemisorption/desorption and TEM/SEM analysis have revealed weak interaction(s) between the Ni crystallites and the aluminosilicate support. An appreciable growth of the supported nickel particles during catalysis was detected and is quantified.