Microwave (MW)-assisted catalytic degradation, being an emerging technique, can potentially fill in the technological gap which promises , prompt, and efficient catalysis, and therefore, suitable MW catalysts are curiously being hunted. Candidature of spinel zinc ferrite (SZFO) atomic sheets as a MW catalyst has thoroughly been investigated in this article. Analytical techniques prove SZFO atomic sheets to be highly crystalline, thermally stable, good dielectric, and superparamagnetic, which render it a potentially strong MW catalyst. Brilliant green (BG) has been demonstrated to be chemisorbed on the SZFO atomic sheets, which upon MW irradiation gets mineralized within 5 min, and the overall efficiency has been observed to be >99%. Total organic carbon removal of ∼80% has been obtained. Ionic chromatography proves the formation of SO and NO anions which increase with MW exposure time. Liquid chromatography mass spectroscopy studies have established intermediate formations during catalysis. SZFO, established as a uniquely suited and highly efficient MW catalyst for BG, is expected to broaden the horizons of MW-assisted catalytic degradation and lead it toward its broader applications.