Methods and systems for optimizing a set of measurement library control parameters for a particular metrology application are presented herein. Measurement signals are collected from one or more metrology targets by a target measurement system. Values of user selected parameters of interest are resolved by fitting a pre-computed measurement library function to the measurement signals for a given set of library control parameters. Values of one or more library control parameters are optimized such that differences between the values of the parameters of interest estimated by the library based measurement and reference values associated with trusted measurements of the parameters of interest are minimized. The optimization of the library control parameter values is performed without recalculating the pre-computed measurement library. Subsequent library based measurements are performed by the target measurement system using the optimized set of measurement library control parameters with improved measurement performance.