The presence of per- and poly-fluoroalkyl substances (PFAS) in soils is a global concern as these emerging contaminants are highly resistant to degradation and cause adverse effects on human and environmental health at very low concentrations. Sequestering PFAS in soils using carbon-based materials is a low-cost and effective strategy to minimize pollutant bioavailability and exposure, and may offer potential long-term remediation of PFAS in the environment. This paper provides a comprehensive evaluation of current insights on sequestration of PFAS in soil using carbon-based sorbents. Hydrophobic effects originating from fluorinated carbon (C–F) backbone “tail” and electrostatic interactions deriving from functional groups on the molecules’ “head” are the two driving forces governing PFAS sorption. Consequently, varying C–F chain lengths and polar functional groups significantly alter PFAS availability and leachability. Furthermore, matrix parameters such as soil organic matter, inorganic minerals, and pH significantly impact PFAS sequestration by sorbent amendments. Materials such as activated carbon, biochar, carbon nanotubes, and their composites are the primary C-based materials used for PFAS adsorption. Importantly, modifying the carbon structural and surface chemistry is essential for increasing the active sorption sites and for strengthening interactions with PFAS. This review evaluates current literature, identifies knowledge gaps in current remediation technologies and addresses future strategies on the sequestration of PFAS in contaminated soil using sustainable novel C-based sorbents.