This work focuses on the site-specific assessment of source zone natural attenuation (SZNA) at petroleum spill sites, including the confirmation that SZNA is occurring, estimation of current SZNA rates, and anticipation of SZNA impact on future ground water quality. The approach anticipates that decision makers will be interested in answers to the following questions: (1) Is SZNA occurring and what processes are contributing to SZNA? (2) What are the current rates of mass removal associated with SZNA? (3) What are the longer-term implications of SZNA for ground water impacts? and (4) Are the SZNA processes and rates sustainable? This approach is a data-driven, macroscopic, multiple-lines-of-evidence approach and is therefore consistent with the 2000 National Research Council’s recommendations and complementary to existing dissolved plume natural attenuation protocols and recent modeling work published by others. While this work is easily generalized, the discussion emphasizes SZNA assessment at petroleum hydrocarbon spill sites. The approach includes three basic levels of data collection and data reduction (Group I, Group II, and Group III). Group I measurements provide evidence that SZNA is occurring. Group II measurements include additional information necessary to estimate current SZNA rates, and group III measurements are focused on evaluating the long-term implications of SZNA for source zone characteristics and ground water quality. This paper presents the generalized site-specific SZNA assessment approach and then focuses on the interpretation of Group II data. Companion papers illustrate its application to source zones at a former oil field in California.