Transforming　spent　coffee　grounds　and　tea　residues　into　valuable　hierarchical　porous　materials　presents　a　sustainable　solution　for　environmental　remediation　due　to　the　low　cost,　extensive　availability,　and　versatile　functionalized　interface.　Here,　we　systematically　investigated　tea　polyphenol-mediated　morphological　transformation　of　spent　coffee　grounds　to　the　synthesis　of　three-dimensional　(3D)　mesoporous　metal-organic　framework　(MOF)-derived　nanoarchitectured　carbon　composites.　We　adopted　the　sustainable　cost-effective　tea-coffee　derivative　to　remove　typical　marine　micropollutants,　such　as　antibiotic　wastewater,　radioactive　pollutants,　and　microplastics.　This　innovative　adsorbent　shows　remarkable　efficiency　in　antibiotic　adsorption,　achieving　up　to　99.62%　removal　of　tetracycline　(TC),　with　an　impressive　maximum　adsorption　capacity　of　373.1　mg/g.　It　also　demonstrates　a　remarkable　ability　to　remove　marine　microplastics　and　radioactive　pollutants　with　immediate　nuclear　threats　and　global　sanitation　and　health　crisis　posed　by　Fukushima　nuclear　waste　toward　the　world.　The　innovative　strategy　of　treating　waste　with　waste　highlights　economic　potential　in　wastewater　treatment.　©　2024　American　Chemical　Society.