Access to safe drinking water remains a critical global challenge, particularly in developing regions and during post-disaster emergencies where conventional water treatment infrastructure is often compromised. This study presents a novel, sustainable, and highly effective point-of-use (POU) water disinfection method utilizing Layered Double Hydroxide (LDH) foils. We addressed key limitations of powdered LDHs by immobilizing them onto aluminum foil, enabling easy application and separation from treated water. A significant innovation lies in replacing hazardous NaOH with safer, more accessible calcium hydroxide (Ca(OH)2) for LDH synthesis, coupled with the exploration of alternative magnesium (Mg) sources like MgCl2, Mg(NO3)2, and Mg(OH)2, which are commonly available as agricultural fertilizers, enhancing local applicability. The synthesized LDH foils underwent characterization using X-ray Diffraction (XRD), confirming successful LDH phase formation. Disinfection efficacy was rigorously evaluated against Escherichia coli (E. coli) as a model pathogen. Results demonstrate remarkable removal efficiency: LDH foils prepared with MgCl2, Mg(NO3)2, and Mg(OH)2, and seawater achieved near-complete E. coli elimination (<1 CFU/mL) within 3 hours, while Mg(OH)2-derived foils also showed significant reduction. This efficient and rapid destruction of pathogens, together with ease of application and green synthesis, positions LDH foils as a possible solution to enhance drinking water resilience within rural communities and in disaster relief efforts. Regeneration protocols will be optimized and performance verified within real-world water matrices in the near future.