The unicellular marine algae, Phaeodactylum tricornutum Bohlin, Cyclotella cryptica Reimann and Cyclotella meneghiniana Kützing (Bacillariophyceae) and Porphyridium aerugineum Geitler (Rhodophyceae) synthesized and accumulated glycine betaine and proline in response to increases of the NaCl concentration (150 to 1000 mol m−3NaCl) of the growth medium. C. cryptica and C. meneghiniana also synthesized and accumulated homarine (N-methyl picolinic acid betaine). Both P. tricornutum and P. aerugineum synthesized increasing amounts of intracellular glycerol and P. aerugineum also formed the heteroside, floridoside [O-α-D-galactopyranosyl (1 → 2)-glycerol], in response to the elevated salinities. No major low molecular weight carbohydrates were found in Cyclotella. Sucrose was not detected in the algal extracts. Only P. tricornutum synthesized the tertiary sulphonium compound, β-dimethylsulphoniopropionate (DMSP), and the quantity of this solute in the alga was dependent on the amount of NaCl in the medium. Intracellular K+concentrations in the algae were three to six times greater than those of Na+. Increases of the salinity of the media led to the uptake and accumulation of K+by the cells, and smaller increases of Na+and Cl−1and loss of intracellular NO3−. The inorganic cations Na+and K+, with their accompanying anions, and the estimated organic solutes could largely account for the osmotic balance of P. tricornutum and P. aerugineum.