Green hydrogen is central to the energy transition, but its production often requires expensive materials and poses environmental risks due to the perfluorinated substances used in electrolysis. This study introduces a transformative approach to green hydrogen production via chemical looping, utilizing an iron-based oxygen carrier with yttrium-stabilized zirconium oxide (YSZ). A significant innovation is the replacement of Al₂O₃ with SiO₂ as an inert support pellet, enhancing process efficiency and reducing CO₂ contamination by minimizing carbon deposition by up to 700%. The major findings include achieving a remarkable hydrogen purity of 99.994% without the need for additional purification methods. The Fe-YSZ oxygen carrier possesses a significantly higher pore volume of 323 mm³/g and pore surface area of 18.3 m²/g, increasing the pore volume in the iron matrix by up to 50%, further improving efficiency. The catalytic system exhibits a unique self-cleaning effect, substantially reducing CO₂ contamination. Fe-YSZ-SiO₂ demonstrated CO₂ contamination levels below 100 ppm, which is particularly noteworthy. This research advances our understanding of chemical looping mechanisms and offers practical, sustainable solutions for green hydrogen production, highlighting the crucial synergy between support pellets and oxygen carriers. These findings underscore the potential of chemical looping hydrogen (CLH) technology for use in efficient and environmentally friendly hydrogen production, contributing to the transition to cleaner energy sources.