A framework for verification and validation/uncertainty quantification of largescale, highly coupled, complex processes is presented. Steps in the framework include code and solution verification, development of an input/uncertainty map, definition of evaluation criteria, development of a surrogate model, performance of a consistency analysis (a mathematical statement limiting error), and the feed forward and feedback of information gain from the analysis. This framework is applied to a turbulent, buoyant, 1 m diameter helium plume. Experimental measurements are obtained from Sandia National Laboratory while the helium plume simulations are performed using Large Eddy Simulation. Both parameter and experimental uncertainty associated with the helium plume are reduced by requiring consistency.