Sugarcane bagasse is the main solid waste of sugar extraction industry. However, there are less eco-friendly treatment methods for this kind of waste material. Most of them have been burned and this is a challenge for effective utilization of sugarcane. Herein, Zn/Co-ZIF nanoparticles are loaded onto the aerogel obtained from bagasse cellulose by doping method to form pomegranate-like structure products, i.e., Zn/Co-ZIF@GEL. By simulating the pomegranate-biomimetic structure, the leaching of cobalt ions is suppressed and enhanced its catalytic activity. Also, Zn/Co-ZIF@GEL behaves outstanding peroxymonosulfate (PMS) activation reactivity to degrade Rhodamine B (RhB) with achieving 100% removal rate in 30 min with enhanced water stability. The outer wrapping of nanoparticles by aerogel exhibits excellent reusability and the removal rate remains above 92% after 4 cycles. X-ray photoelectron spectroscopy (XPS) verifies the electron transfer between the heterostructures of Zn and Co could ensure the catalyst continues to complete the redox cycle with synergistic effect. Electron paramagnetic resonance (EPR) further investigates the non-radical singlet oxygen is the predominant degradation pathway of RhB. This work provides a new strategy for improved bagasse derivate ZIF catalytic application.