As high-density polyethylene (HDPE) geomembranes in landfill liner systems increasingly age and damage, seepage incidents frequently occur and severely threaten the surrounding ecological environment and groundwater safety. Targeted injection grouting with polymer materials can rapidly restore the barrier function by repairing defects in damaged geomembranes. To investigate the sealing mechanisms of polymer grouting bodies with various densities, this study used low-field nuclear magnetic resonance (LF NMR) techniques to monitor and visualize the permeation process within the grouting bodies. The results revealed two failure modes of the grouting bodies under water flows: 1) insufficient interfacial shear strength between the low-density polymer and geomembrane, leading to interfacial leakage; 2) gradual buildup of permeation pressure puncturing the foam cells of the polymer matrix and inducing permeation channels. Selecting polymers with suitable expansion ratios to produce appropriate expansive pressures is crucial to enhance interfacial shear strength while avoiding secondary damages to geomembranes. Increasing the density of the polymer grouting body can also enhance the compressive strength of foam cells and interfacial shear resistance. These are crucial for enabling grouting repair of defects in geomembranes and improving their barrier performance.