The widespread issue of microplastic pollution in aquatic environments has garnered international attention because of its detrimental effects on the environment and human health. Utilizing the remarkable qualities of carbon-based materials such as graphene, carbon nanotubes (CNTs), and graphene oxide (GO), carbon-based nanocomposites have emerged as novel techniques to address this issue. These materials are perfect for the adsorption and degradation of microplastics because of their large surface area, adjustable surface chemistry, and exceptional mechanical and chemical stability. This chapter examines the types, designs, techniques, and applications of carbon-based nanocomposites in the removal of microplastics. This chapter also covers important mechanisms, such as advanced oxidation processes (AOPs), which break down microplastic polymers into smaller, less dangerous compounds, and adsorption powered by van der Waals forces and hydrophobic contacts. Apart from discussing the processes of oxidative, photocatalytic, and enzymatic degradation, this chapter emphasizes the benefits of nanomaterials in the disintegration of different types of microplastics and their use in both lab and real-world environments. This chapter also discusses the safety concerns, environmental impacts, and possible uses of nanoparticles, including new types and scalability challenges. To sum up, a comprehensive analysis of the issue’s mechanics and insights was offered, which could improve the efficiency of catalytic techniques for removing these microplastics.