Department of Energy (DOE) facilities within the weapons complex face a daunting challenge of remediating huge below inventories of legacy radioactive and toxic metal waste. More often than not, the scope of the problem is massive, particularly in the high recharge, humid regions east of the Mississippi river, where the off-site migration of contaminants continues to plague soil water, groundwater, and surface water sources. As of 2002, contaminated sites are closing rapidly and many remediation strategies have chosen to leave contaminants in-place. In situ barriers, surface caps, and bioremediation are often the remedial strategies of chose. By choosing to leave contaminants in-place, we must accept the fact that the contaminants will continue to interact with subsurface and surface media. Contaminant interactions with the geosphere are complex and investigating long term changes and interactive processes is imperative to verifying risks. We must be able to understand the consequences of our action or inaction. The focus of this presentation is to describe recent technical developments for assessing the performance of in situ bioremediation and immobilization of subsurface metals and radionuclides. Research within DOE's NABIR and EMSP programs has been investigating the possibility of using subsurface microorganisms to convert redox sensitive toxic metals and radionuclides (e.g. Cr, U, Tc, Co) into a less soluble, less mobile forms. Much of the research is motivated by the likelihood that subsurface metal-reducing bacteria can be stimulated to effectively alter the redox state of metals and radionuclides so that they are immobilized in situ for long time periods. The approach is difficult, however, since subsurface media and waste constituents are complex with competing electron acceptors and hydrogeological conditions making biostimulation a challenge. Performance assessment of in situ biostimulation strategies is also difficult and typically requires detailed monitoring of coupled hydrological, geochemical/geophysical, and microbial processes. In the following presentation we will (1) discuss contaminant fate and transport problems in humid regimes, (2) efforts to immobilize metals and radionuclides in situ via bioremediation, and (3) state-of -the-art techniques for assessing the performance of in situ bioreduction and immobilization of metals and radionuclides. These included (a) in situ solution and solid phase monitoring, (b) in situ and laboratory microbial community analysis, (c) noninvasive geophysical methods, and (d) solid phase speciation via high resolution spectroscopy.