Firefighters are uniquely exposed to per- and polyfluoroalkyl substances (PFASs) from use of aqueous film-forming foam (AFFF) and potentially from PFASs-treated turnout gear. This study assessed firefighter’s ambient (nondietary) exposure to PFASs using silicone wristbands. Twenty-three firefighters from North Carolina wore a new wristband during each 9-day work period for approximately 4 months. While wearing the wristbands, each firefighter reported on fire calls using an App installed on their phones. Wristbands, and blood plasma samples collected at study completion, were analyzed for PFASs. PFASs were detected in all blood samples and were dominated by TFA, PFOA, PFOS, PFPrA and PFHxS. Several PFASs levels were positively associated with age and years as a firefighter. Analytes commonly detected in wristbands were MeFBSE, MeFOSE, PFHxA, PFUnA, 6:2 diPAP, 8:2 diPAP, and 6:2/8:2 diPAP. Wristband MeFBSE levels were associated with the number of fires and duration of time spent at a fire. MeFOSE levels on wristbands were also significantly and positively correlated with plasma N-MeFOSAA, similar to a previous study in a nonfirefighter cohort. Overall, these findings suggest that silicone wristbands can detect some occupational PFASs exposures among firefighters and highlights the potential for specific PFASs compounds to be associated with firefighting activities.