Controlling leakage and infiltration in subsurface is critical for maintaining underground structural stability and mitigating environmental impacts. Conventional cement-based grouts have high CO2 emissions and the potential for internal discontinuities. This study investigated the applicability of biopolymer-based grout systems, including xanthan gum grout, agar gum grout, gelatin grout, and gelatin-tannic acid grout, as sustainable alternatives to conventional cement grout. Scaled geotechnical models featuring various structures, including H-core, Double H-core, Secant-Construction in Place (CIP), and Trapezoid-core, were subjected to high-pressure (up to 500 kPa) permeability tests to assess their impermeability and injection performance. The pre-treatment hydraulic conductivity ranged from approximately 10-8 to 10-5 cm/s, whereas post-treatment values after 1-7 days of curing decreased to approximately 10-9-10-6 cm/s for most biopolymer-treated specimens. Among the tested materials, gelatin-tannic acid grout showed the most pronounced short-term permeability reduction due to crosslinking-enhanced gel formation. In particular, crosslinked gelatin with tannic acid produced robust gel networks, ensuring favorable impermeability under high-pressure conditions. Injectability tests showed that agar gum exhibited higher initial injection volumes due to its low viscosity, while smaller amounts of xanthan gum achieved comparable permeability reductions, underscoring economic and environmental advantages. By contrast, although cement grout offers a low unit material cost, its large-scale use significantly increases CO2 emissions and can re-initiate leakage pathways through internal discontinuities during prolonged high-pressure injection. Overall, these findings demonstrate the potential of biopolymer-based grouts for short-term permeability reduction in scaled geotechnical structures. However, long-term durability, biodegradation resistance, cyclic hydraulic loading, and field-scale validation should be further investigated before practical implementation.