An accurate conceptual site model (CSM) and plume‐delineation at contamination sites are pre‐requisites for successful remediation and for satisfying regulators and stakeholders. PlumeSeeker™ is well‐suited for assessing data gaps in CSMs by using available site data and for identifying the optimal number and locations of sampling locations to delineate contaminant plumes. It is an enhancement of a university research code for plume delineation using geostatistical and stochastic modeling integrated with the groundwater modeling software MODFLOW‐SURFACT™. PlumeSeeker™ increases the overall confidence in the location of the plume boundary through a variance‐reduction approach that selects existing‐ or new monitoring wells for sampling based on minimizing the uncertainty in plume boundary and on new field information. Applicable at sites with or without existing monitoring wells, PlumeSeeker™ is particularly powerful for optimally allocating project resources (labor, well installation, and laboratory costs) between existing wells and sampling at new locations. An application of PlumeSeeker™ at Lakehurst, the naval component of Joint Base McGuire‐Dix‐Lakehurst in New Jersey, demonstrates how the cost of delineating the migration pathway of a perfluorooctanoic acid (PFOA) plume can be minimized by requiring only 9 new sampling locations in addition to samples from 2 existing wells for achieving a 70% reduction in plume uncertainty. In addition, the use of available site data in three different scenarios identified CSM data‐gaps in the source area and in the interaction between Manapaqua Branch and groundwater, where the observed high concentration in this area could have resulted from a combination of groundwater migration and induced infiltration.