An efficient, green and reusable catalyst for organic pollutant wastewater treatment has been a subject of intense research in recent decades due to the limitation of current technologies. Cellulose based aerogel composites are considered to be an especially promising candidate for next-generation catalytic material. This project was conducted in order to evaluate the behavior and ability of green and reusable sugarcane bagasse aerogels to remove P-Nitrophesnol from waste-water aqueous. Co-Zeolitic imidazolate framework@ sugarcane bagasse aerogels composite catalysts were successfully prepared via simple in situ synthesis. The structure of hybrid aerogels and their efficient catalyst in peroxymonosulfate (PMS) activation for the degradation of p-nitrophenol (PNP) was investigated. As a result, the hybrid aerogels/PMS system removed 98.5% of PNP (10 mg/L) within 60~70 min, while the traditional water treatment technology could not achieve this. In addition, through a free radical capture experiment and electron paramagnetic resonance (EPR), the degradation mechanism of PNP was investigated. Further research found that the hybrid aerogels can effectively activate PMS to produce sulfate (SO∙ −4) and hydroxyl (OH∙ ). Both of them contributed to the degradation of PNP, and SO∙ −4 plays a crucial role in the degradative process. The most important feature of hybrid aerogels can be easily separated from the solution. The obtained results showed that the outer coating structure of cellulose can stabilize Co-ZIF and reduce the dissolution of cobalt ions under complex reaction conditions. Moreover, the prepared hybrid aerogels exhibit excellent reusability and are environmentally friendly with efficient catalytic efficiency. This work provides a new strategy for bagasse applications and material reusability.