Hierarchically porous graphitic aerogels (HGAs) are gaining attention as versatile platforms for applications spanning water purification, electromagnetic interference shielding, energy storage, and environmental remediation. Yet, the synthesis of such materials often relies on multi-step fabrication techniques involving separate processes for carbonization/graphitization and structure formation, which can hinder scalability and material tunability. In this work, we introduce a streamlined pyrolytic approach that capitalizes on the intrinsic foaming behavior of proteins to produce monolithic aerogels featuring interconnected sheet- and fiber-like morphologies, with ultralow densities (~3 mg/cm³). This template-free process requires no harsh chemicals or post-synthesis treatments. As a proof of concept, we demonstrate the application of the resulting HGA as an anode material in microbial electrolysis cells (MECs) for simultaneous degradation of perfluorooctanoic acid (PFOA) and oxidation of ammonium by Acidimicrobium Strain A6, which has been shown to degrade PFOA, including in MECs. The HGA anode achieves complete ammonium removal and over 99% PFOA degradation, outperforming conventional anodes in both current density and pollutant conversion efficiency. This work presents a cohesive processing-structure-function strategy for the development of tunable, sustainable carbon architectures, offering a promising solution for wastewater treatment and environmental remediation.
