Carbon nanotubes have been synthesised by catalytic chemical vapour deposition of a H₂–CH₄ mixture (18 mol% CH₄) over (Mg,Co,Mo)O catalysts. The total amount of cobalt and molybdenum has been kept constant at 1 cat% and the proportion of molybdenum with respect to cobalt has been varied from x(Mo) = 0.25–1.0. This variation has important effects on both the yield and the nature (number of walls, straight walls or bamboo-like structures) of the carbon nanotubes. It also has an influence on the purity of the samples (amount of encapsulated metal particles, presence or not of amorphous carbon deposits). For x = 0.25, the nanotubes were mainly double- and triple-walled (inner diameter less than 3 nm); samples prepared from catalysts with higher molybdenum ratios contained larger multi-walled carbon nanotubes (inner diameter up to 9 nm), having up to 13 concentric walls. It is proposed that different growth mechanisms may occur depending on the initial composition of the catalyst.