The cause of feline hyperthyroidism (FH), a common endocrinopathy of domestic cats, is unknown. A potential association between exposure to environmental contaminants polybrominated diphenyl ethers (PBDEs) and FH was investigated. The median serum level for the sum of congeners BDE-47, BDE-99, BDE-153, BDE-154 and BDE-183 (Σ5) in hyperthyroid and euthyroid cats was 82 and 174 ng g−1 lw respectively with no significant difference in PBDE levels or profiles between groups. Overall, the median (min to max) concentration of PBDEs in cat serum (n=65) was 118 ng g−1 lw (5–5260 ng g−1 lw), which is approximately 10 times higher than that observed in the Australian human population. Furthermore, congener composition in feline serum samples was dominated by congener BDE-99, followed by BDE-47 then BDE-153 which differs from results of human biomonitoring. There was no correlation between PBDE levels in feline serum samples and matched house dust samples (n=25). However the similarity of BDE-47/99 ratio in each matrix suggests dust is likely the dominant exposure. Calculation of the daily exposure dose via dust ingestion for cats equated to a mean of 33 ng kg−1 bw d−1 (0.2–150 ng kg−1 bw d−1). Differences in exposure estimates for Australian and US cats, based on dust ingestion alone, are consistent with the observed differences in body burdens. Our results do not support a role for PBDE exposure in the aetiopathogenesis of FH.