Carbon nanotube membranes (CNMs) were prepared by doing chemical vapor deposition of carbon within the pores of a microporous alumina template. Electroosmotic flow (EOF) was driven across the CNMs by allowing the membrane to separate two electrolyte solutions and using an electrode in each solution to pass a constant ionic current through the nanotubes. EOF was investigated by measuring the flux of a probe molecule (phenol) across the CNM. The as-synthesized CNMs have anionic surface charge, and EOF is in the direction of cation migration across the membrane. Measurements of the rate of EOF as a function of applied transmembrane current provided the zeta potential. The effect of pH on zeta provided the pK(a) for the surface acidic sites responsible for this anionic charge; the acidic-site density was also determined. An electrochemical derivatization method was used to attach carboxylate groups to the nanotube walls; this enhances the anionic surface charge density, resulting in a corresponding increase in the EOF rate. Electrochemical derivatization was also used to attach cationic ammonium sites to the nanotube walls to yield CNMs that show EOF in the opposite direction of the as-synthesized or carboxylated membranes.