The response of cats to dietary sodium selenite (Na2SeO3) and organically bound selenium was studied in two separate studies with four cats per treatment and three levels of selenium supplementation (targets 1.0, 1.5 and 2.0 μg/g DM) for each Se source. Whole blood and plasma selenium concentrations and glutathione peroxidase (GPx) activity were determined at 7-time points across the 32-day study. Faeces were quantitatively collected during the last 8 days and urine was collected daily during both studies. The basal diet used had a low apparent faecal selenium absorption of 25.3 ± 3.0%. Daily faecal and urinary selenium excretion increased linearly with increasing selenium intake for both Se sources. Urinary selenium concentration of the cats fed the supplemented diets increased rapidly (∼2 days) and remained constant throughout the remainder of the study. Apparent faecal selenium absorption was high for both selenium sources (73.2% and 80.0%). Plasma, and to a lesser extent, whole blood selenium concentrations increased in a dose-dependent manner with supplementation. Whole blood and plasma GPx activity were highly variable and showed a variable response to dietary selenium intake. Cats closely regulate selenium homeostasis through increasing urinary excretion whilst faecal absorption remains unaffected.