Metal-organic frameworks (MOFs) are one of the most promising advanced heterogeneous catalysts for the activation of peroxymonosulfate (PMS) to degrade organic contaminants in water, and have been extensively studied.However, MOFs in powder form usually have the disadvantage of poor separation and regeneration, making it significantly challenging for practical applications. In this study, ultralight zeolitic imidazolate framework-67@poly(vinyl alcohol)/citric acid nanofibrous aerogel (ZIF-67@PVA/CA NFA) was prepared by a convenient and facile in-situ growth method and it had excellent catalytic efficiency and recyclability. The factors affecting the activation of PMS by ZIF-67@PVA/CA NFA, such as PMS concentration, reaction temperature, solution pH, and organic pollutant concentration, were investigated. Taking advantage of the distinctive structural characteristics of MOF and nanofibrous aerogels, the obtained ZIF-67@PVA/CA NFA exhibited ultralow density, hierarchical porosity, remarkably high catalytic activity for activation of PMS for the degradation of organic pollutants. Furthermore, ZIF-67@PVA/CA NFA also displayed excellent recyclability along with retention of high catalytic stability.The present study provides a new strategy for the efficient fabrication of threedimensional heterogeneous catalyst for the activation of PMS, with great potential in wastewater treatment.