Phosphorus recovery from sanitary wastewater is critical for sustainable agriculture and environmental protection. This research presents an innovative approach combining material synthesis and chemometric optimization to develop a robust, cost-effective solution for phosphorus capture. A composite material, SiO2@FeOOH, derived from quartz sand waste and scrap iron, was synthesized via a green, scalable coprecipitation method. The process was optimized using Design of Experiments (DoE) to enhance phosphorus adsorption capacity while adhering to zero-waste principles. The optimized adsorbent exhibited a high phosphorus adsorption capacity (up to 40 mg P/g) and resilience under conditions simulating treated wastewater, including the presence of competing ions and humic substances. Chemometric modeling elucidated the impact of synthesis parameters on the material’s properties, enabling precise control of its performance. Key findings revealed that the presence of calcium ions enhanced phosphorus capture by forming insoluble calcium-phosphorus deposits, while maintaining the adsorbent’s regeneration potential. This work highlights a dual achievement: turning industrial waste into a value-added product and advancing circular economy practices in wastewater treatment. The combination of sustainable synthesis and chemometric insights underscores the potential for scalable phosphorus recovery technologies, addressing both environmental and agricultural challenges. These results align with global sustainability goals, offering a pathway to integrate waste management with nutrient recycling effectively. Therefore, this work explores the synthesis process, chemometric strategies, and environmental implications of this approach, emphasizing its alignment with innovation startegies in sustainable waste management.