Sulfate radical-based advanced oxidation processes (SR-AOPs) is a very efficient wastewater treatment technology and has great potential for environmental remediation. However, finding efficient catalysts for activation of peroxomonosulfate (PMS) is still challenge. In this work, we synthesized a ZIF-67-coated natural sponge composite (ZS) using the in-situ growth method, and the material obtained after carbonization (ZSC) was used to activate PMS for better removal of 4-nitrophenol (4-NP). Natural sponges as carriers for loaded MOF materials can better stimulate the ability of composites to activate PMS, for example: (1) Prevents deactivation of MOF particles due to the occurrence of aggregation; (2) Solves the problems caused by the powder characteristics of the MOF particles themselves, prevents secondary contamination, and is easy to recycle; (3) Limit the risk of loss of MOF particles. The removal efficiency of ZSC-activated PMS for 4-NP (10 ppm) was remarkable at 99 %. Natural sponges as carriers, are taken from the natural environment, which is more affinity with the environment, reduces the risk of pollution and highlights the sustainability of the material. This study proposes a green and sustainable material for the removal of 4-NP to provide technical support for water ecological management