The behaviour of iodine in the environment is of interest both in relation to radioecology and human nutrition. Radiochemical techniques were used to evaluate various aspects of the behaviour of iodine in the environment. The natural iodine content of plant, water and soil samples collected from three sites was determined using preconcentration neutron activation analysis (PNAA). The effect of initial chemical speciation on the distribution of iodine between various soils, sediments and waters was evaluated using I-131 tracer. Iodide was found to adsorb more extensively than iodate, although for most of the solid/water systems examined, a substantial portion of the iodate was slowly reduced to iodide. Experiments involving gamma irradiation suggest that much of the sorption of iodide and reduction of iodate involved microbial processes. Distribution coefficients measured using I-131 were comparable with values based on the natural I-127 content.