Ion movements associated with the pH rise that is observed upon illumination of thylakoid suspensions at low pH have been studied by a multiparameter technique. Light-dependent, dark-reversible fluxes of H(+), Cl(-), Na(+), K(+) and divalent cations were monitored, together with simultaneous changes in the optical density of the suspension. Extensive uptake of Cl(-) and efflux of Mg(2+) accompany the apparent inward movement of H(+) in the light. Only minor efflux of K(+) is seen and Na(+) appears immobile. The Cl(-) and Mg(2+) fluxes together compensate for most of the charge transferred as H(+), contributing respectively about 49% and 43% on an equivalent basis. The ratio of Cl(-) influx to Mg(2+) efflux is variable, but usually >1.0. The Mg(2+) flux can be supplanted by (1) K(+) flux, if the K(+)/Mg(2+) activity ratio in the suspension is high, and (2) Ca(2+) flux, if the thylakoids are equilibrated with suspending media containing Ca(2+). The affinity of the divalentcation-binding sites, or carrier mechanism, is greater for Ca(2+) than for Mg(2+). Schemes can be drawn up to account for the observed ion movements on the basis of either a chemical or a chemiosmotic mechanism for energy transduction in chloroplasts. In intact chloroplasts, light-dependent control of Mg(2+) distribution between thylakoid and stroma could serve to regulate enzyme activities in the carbon fixation pathway, and hence photosynthesis.