Inorganic carbon transport was investigated in a range of marine microalgae. A small-celled strain of Stichococcus bacillaris, containing appreciable carbonic anhydrase activity, showed a high affinity for CO2, while measurement of the internal inorganic carbon pool by the silicone oil layer centrifugal filtering technique showed cells concentrated inorganic carbon up to 20-fold in relation to the external medium at pH 5.0 but not pH 8.3. The addition of 14CO2 or H14CO3− to cells in short-term kinetic experiments at pH 8.3 confirmed that only CO2 provides the exogenous substrate for substantial inorganic carbon accumulation within the cell. High-affinity HCO3− transport in Phaeodactylum tricornutum and Porphyridium purpureum is dependent on sodium ions, while intracellular carbonic anhydrase increased the steady-state flux of CO2 from inside the plasmalemma to Rubisco. In the presence of HCO3− the intracellular pH in cells of P. purpureum is 7.1 but on carbon starvation the pH falls to 6.0. Ethoxyzolamide blocks bicarbonate-dependent alkalinization of the cytosol, confirming a central role for carbonic anhydrase–bicarbonate in cytosolic pH regulation. Carbonic anhydrase activity is pH dependent in P. purpureum so synergistic interaction between CO2 uptake and bicarbonate transport may occur.