Contaminate-sequestering coatings including a network of hydrolyzed silane compounds including a plurality of thiol functional groups, a plurality of fluorinated functionalities, or both are provided. The contaminate-sequestering coatings may sequester one or more per- and polyfluoroalkyl substances (PFAS), heavy metals, biological species or any combination thereof. Methods of functionalizing a substrate surface with contaminate-sequestering functionalities that sequester one or more PFAS, heavy metals, or both are also provided. Methods of removing contaminants from contaminate-containing liquids, and devices including the contaminate-sequestering coatings are also provided.