Wastewater is an important source of perfluoroalkyl acids (PFAAs) to environmental waters. PFAAs are poorly removed during conventional wastewater treatment and only moderately removed by nonselective adsorbents [e.g., activated carbon (AC)]. Molecularly imprinted polymers (MIPs) enable selective adsorption of trace organics (e.g., PFAAs) by templating polymerization with a target compound; however, MIP morphology limits use for wastewater treatment. To overcome this obstacle, a perfluorooctanesulfonate (PFOS)-templated MIP was immobilized on spent coffee grounds biochar�an eco-friendly AC alternative�via radical initiated polymerization. Vinylbenzyl trimethylammonium chloride (VBTAC) and/or 2-(trifluoromethyl)acrylic acid served as functional monomers for MIP synthesis. First, biochar surfaces were functionalized with −NH MIP attachment points via (i) electrophilic aromatic substitution followed by reduction or (ii) heat-catalyzed addition of melamine. Melamine-modified biochar functionalized with VBTAC-MIP