TOC abstract (IMAGE) Shanghai Jiao Tong University Journal Center Caption A series of sulfides/carbon composites with sulfur vacancies-rich sulfides heterointerfaces are well-designed and developed via a simple one-pot carrageenan-assistant cations-regulated strategy. “Janus effect” of interfacial sulfur vacancies, which triggers strong defect-type interfacial polarization, are firstly intuitively confirmed by both theoretical and experimental investigations. Optimized Co/Ni-carbon composites (CAs) imbued with sulfur vacancies-rich heterointerfaces displays broad absorption bandwidth of 6.76 GHz at only 1.8 mm, compared to sulfur vacancies-free CAs without any dielectric response. Credit All authors Usage Restrictions Credit must be given to the creator. Only noncommercial uses of the work are permitted. No derivatives or adaptations of the work are permitted. License CC BY-NC-ND Disclaimer: AAAS and EurekAlert! are not responsible for the accuracy of news releases posted to EurekAlert! by contributing institutions or for the use of any information through the EurekAlert system.