Microplastics (MPs) pollution in household wastewater and global aquatic systems has become an emerging issue and potential threat to marine life and human health. However, advanced technologies for efficient MPs control and purification remain largely underdeveloped. Herein, we present integrated carbocatalytic oxidation and hydrothermal (HT) hydrolysis of microplastics over magnetic spring-like carbon nanotubes. The robust carbon hybrids exhibited an outstanding MPs degradation performance by catalytic activation of peroxymonosulfate to generate reactive radicals. The spiral architecture and highly graphitic degree guaranteed the superb stability of the carbocatalysts in HT environment. The toxicity tests indicated that the organic intermediates from MPs degradation were environmentally benign to the aquatic microorganisms and can serve as a carbon source for algae cultivation. The outcomes of this study are dedicated to providing a green strategy by integrating state-of-the-art carbocatalysis and nanotechnology for remediation of MPs contamination in water.