ABSTRACT Global public health concern is growing over per- and polyfluoroalkyl substances (PFASs) toxicity, environmental persistence, and potential to bioaccumulate in humans and wildlife. Nearly every person who has been tested for PFASs shows measurable levels in their blood resulting from contamination of the environment and continued use in consumer products and industrial applications. In particular, drinking water appears to be the major source of PFAS exposure for people living near contaminated sites. Importantly, some PFASs have been linked to liver damage, developmental impacts, and several cancers (e.g., kidney, testicular). Environmental remediation is urgently needed, but efforts are hampered by the extreme persistence of the carbon-fluorine bond. Biodegradation typically involves only the non-fluorinated components of polyfluorinated PFASs, resulting in the creation of shorter-chain perfluorinated acids that are more persistent and mobile. Complete mineralization has not been demonstrated. Abiotic treatment technologies can be more effective but require extremely high energy inputs, and the degradation mechanisms are poorly understood. There is a critical need for a treatment technology with lower energy requirements, and for enhanced degradation pathways that efficiently mineralize PFASs without formation of perfluorinated acids that persist after treatment. The overarching goal of this proposal is to develop an innovative nanomaterial-biological strategy to tackle the challenge of PFAS biodegradation. Our central hypothesis is that pretreatment by tailored nanomaterials can facilitate transformation of structurally diverse PFASs to achieve more efficient and complete biodegradation. Our previous work has shown that functionalized nanohybrid catalysts incorporating reduced graphene oxide (rGO) and nano zerovalent iron (nZVI) can successfully initiate degradation of long-chain PFASs. Here, we will employ this abiotic transformation as an innovative pretreatment to unlock the biodegradation of PFASs. Leveraging our expertise in molecular modeling and ‘omics’ techniques, we will test and tailor the ability of microbial communities to more efficiently degrade pretreated PFASs and their initial degradation products. All degradation products will be characterized by high-resolution mass spectrometry and 19F-nuclear magnetic resonance spectroscopy to reveal the mechanisms that enable this nano-bioremediation strategy. This research will tackle a pressing environmental contamination problem with three complementary specific aims: Aim 1: Synthesize multifunctional redox-active nanohybrid materials and evaluate their catalytic properties for PFAS degradation (dehalogenation, degradation of long-chains to short-chains). We will synthesize and characterize two multifunctional and hierarchical carbon-metal nanohybrids: (i) redox-active reduced graphene oxide nano zerovalent iron (rGO–nZVI) and (ii) photocatalytic rGO-nZVI- titanium dioxide (...