Polyfluoroalkyl substances, particularly perfluorooctane sulfonate (PFOS), are persistent environmental pollutants with severe health risks due to their bioaccumulation and resistance to degradation. Current PFOS removal technologies are limited by either efficiency, cost, or environmental concerns. Here, we introduce a biocompatible, protein-based sponge approach using bovine serum albumin (BSA) as a scaffold for efficient PFOS removal. We developed highly porous, mechanically robust sponges by optimizing foaming parameters such as mixing speed, duration, and surfactant concentration. Advanced characterization techniques, including microcomputed tomography and cryo-scanning electron microscopy, confirmed the sponges' structural integrity. Leveraging natural BSA-PFOS interactions, the sponges demonstrate effective PFOS removal, achieving up to ≈80% efficiency at a pH of ≈7.4, similar to natural water systems. Adsorption behavior is described using Langmuir and Freundlich isotherms, showing high adsorption capacity and surface interaction. Mechanical testing confirmed durability, making the sponges suitable for real-world applications. This eco-friendly method surpasses conventional PFOS removal techniques, offering a cost-effective solution with potential applications in drug delivery, tissue engineering, and catalysis. This work paves the way for developing multifunctional, porous protein-based materials that address urgent environmental challenges while offering versatile applications in biotechnology.