We consider the problem of providing optimal uncertainty quantification (UQ) – and hencerigorous certification – for partially-observed functions. We present a UQ frameworkwithin which the observations may be small or large in number, and need not carryinformation about the probability distribution of the system in operation. The UQobjectives are posed as optimization problems, the solutions of which are optimal boundson the quantities of interest; we consider two typical settings, namely parametersensitivities (McDiarmid diameters) and output deviation (or failure) probabilities. Thesolutions of these optimization problems depend non-trivially (even non-monotonically anddiscontinuously) upon the specified legacy data. Furthermore, the extreme values are oftendetermined by only a few members of the data set; in our principal physically-motivatedexample, the bounds are determined by just 2 out of 32 data points, and the remaindercarry no information and could be neglected without changing the final answer. We proposean analogue of the simplex algorithm from linear programming that uses these observationsto offer efficient and rigorous UQ for high-dimensional systems with high-cardinalitylegacy data. These findings suggest natural methods for selecting optimal (maximallyinformative) next experiments.