Feline hyperthyroidism is the most commonly diagnosed endocrine-related disease among senior and geriatric housecats, but the causes remain unknown. Exposure to endocrine-disrupting compounds with thyroid targets, such as flame retardants (FRs), may contribute to disease development. Silicone passive sampling devices, or pet tags, quantitatively assessed the bioavailable FR exposures of 78 cats (≥7 y) in New York and Oregon using gas chromatography-mass spectrometry. Pet tags were analyzed for 36 polybrominated diphenyl ethers, six organophosphate esters (OPEs), and two alternative brominated FRs. In nonhyperthyroid cats, serum free thyroxine (fT4), total T4 (TT4), total triiodothyronine, and thyroid-stimulating hormone concentrations were compared with FR concentrations. Tris(1,3-dichloro-2-isopropyl) phosphate (TDCIPP) concentrations were higher in hyperthyroid pet tags in comparison to nonhyperthyroid pet tags (adjusted odds ratio, p < 0.07; Mantel-Cox, p < 0.02). Higher TDCIPP concentrations were associated with air freshener use in comparison to no use (p < 0.01), residences built since 2005 compared to those pre-1989 (p < 0.002), and cats preferring to spend time on upholstered furniture in comparison to no preference (p < 0.05). Higher TDCIPP concentrations were associated with higher fT4 and TT4 concentrations (p < 0.05). This study provides proof-of-concept data for the use of silicone pet tags with companion animals and further indicates that bioavailable TDCIPP exposures are associated with feline hyperthyroidism.