Sustainable remediation has been increasingly regarded as a promising alternative in recent years. It considers
net environmental impacts
such as energy use, greenhouse gas emission, and waste reduction. Passive
in situ
remediation or natural attenuation are the key component of sustainable remediation often intended to minimize the net environmental impacts. However, leaving contaminants in the subsurface requires the increased burden of proof to show that plumes are stable and residual contaminants do not pose a significant health risk. Particularly in complex geological environments and for actinide species with complex geochemical behaviors, it is difficult to ensure the system stability as well as to predict the future plume conditions. This article presents recent scientific advances to support sustainable remediation in complex geological systems, including site characterization techniques, hydrological and geochemical model developments, and numerical simulations. In particular, we highlight the recent developments in non‐invasive geophysical characterization as well as computationally efficient geochemical models for describing uranium and other reactive species. We demonstrate this approach using the extensive data and models from the Savannah River Site F‐area, which has been contaminated by low‐level radioactive waste solutions including uranium, tritium, and other radionuclides.