The integration of renewables into electrical grids calls for optimization-based control schemes requiring reliable grid models. Classically, parameter estimation and optimization-based control is often decoupled, which leads to high system operation cost in the estimation procedure. The present work proposes a method for simultaneously minimizing grid operation cost and optimally estimating line parameters based on methods for the optimal design of experiments. This method leads to a substantial reduction in cost for optimal estimation and in higher accuracy in the parameters compared with standard Optimal Power Flow and maximum-likelihood estimation. We illustrate the performance of the proposed method on a benchmark system.