Microbial fuel cells (MFCs) are a promising technology that directly converts organic matter (OM) in wastewater into electricity while simultaneously degrading contaminants. However, MFCs are insufficient for the removal of nitrogenous compounds. Therefore, the post-treatment of MFCs is essential. This study was the first to use natural zeolite adsorption integrated with photosynthesis (ZP) for post-treating MFCs. In this system, no external energy was required; instead, natural light was used to promote the growth of photosynthetic microorganisms, thereby enhancing contaminants removal through the photosynthesis process. To assess the effectiveness of the method, comparisons were conducted under two conditions: dark (no photosynthesis) and light (with photosynthesis). In darkness, extending hydraulic retention time (HRT) enhanced COD and BOD removal by 19.8% and 28.9%, respectively. When exposed to natural light, improvements were even more notable, with COD and BOD removal reaching 32% and 40%, respectively. In both conditions, the method effectively removed NH4 +, achieving 60% efficiency in darkness and 84.5% in light. This study showed that the adsorption capacity of the zeolite reached saturation when the cumulative liquid volume per unit weight of the zeolite exceeded 0.2 L g-1. The key functional photosynthetic microbes were investigated using 16S rRNA and 18S rRNA. This revealed the presence of microorganisms such as Chlorobium, Acidovorax, Novosphingobium, and Scenedesmus, which likely play a role in enhancing the efficiency of photosynthesis in removing contaminants. The study findings indicated that the integration of MFCs-ZP represents an eco-friendly approach capable of resource recovery from wastewater while also meeting discharge standards.