For robot-assisted assembly of complex optical systems, the alignment is facilitated by an accurate pose estimation of its components. However, wavefront-based pose estimation is typically ill-conditioned due to the inherent geometry of conventional industrially manufactured optical components. Therefore, we propose a novel approach in this paper to increase wavefront-based pose estimation accuracy via the design of freeform optics. For this purpose, an optimization problem is derived that parameterizes the component's surfaces by a predetermined freeform surface model. To show the efficacy of our approach, we provide simulation results to compare the pose estimation accuracy for a variety of optical designs. As an application example for the resulting improved pose estimation, a hand-eye calibration of a wavefront sensor is performed. This calibration originates from the field of robotics and represents the identification of a sensor coordinate system with respect to a global reference frame. For quantitative evaluation, the calibrating results are first presented with the aid of simulation data. Finally, the practical feasibility is demonstrated using a conventional industrial robot and additively manufactured freeform lenses.