The chemical modification of multi-walled carbon nanotubes using electrolysis is described. It is found that the evolution of the halogens chlorine or bromine on an anode made from a foil of carbon nanotubes couples halogen atoms to the nanotube lattice. Furthermore, oxygen bearing functional groups. such as hydroxyl and carboxyl groups, are formed at the same time aiding solvation of the nanotubes in water or alcohol without any surfactant. Impurities and low grade modified nanotubes remain insoluble. The halogenated carbon nanotubes can be converted with sodium amide or triphenylmethyllithium to add the corresponding functional groups.