Microwave (MW)-assisted catalytic degradation, being an emerging technique, can potentially fill in the technological gap which promises on-demand, 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 SO4 2- and NO3 - 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.