In this thesis, two aspects of control theory, namely controllability and optimal control, are applied to quantum systems. The presented results are based on group theoretical techniques and numerical studies. By Lie-algebraic analysis, the controllability properties of systems with an arbitrary topology are described and related to the symmetries existing in these systems. We find that symmetry precludes full controllability. Our work investigates well-known control systems and gives rules for the design of new systems. Furthermore, theoretical and numerical concepts are instrumental to...