A method for ab initio structure factor retrieval from large-angle rocking-beam electron diffraction data of thin crystals is described and tested with experimental and simulated data. No additional information, such as atomicity or information about chemical composition, has been made use of. Our numerical experiments show that the inversion of dynamical scattering works best, if the beam tilt range is large and the specimen not too thick, because for moderate multiple scattering, the large tilt amplitude effectively removes local minima in this global optimization problem.