This volume contains the proceedings of a Leiden Workshop on Dynamical Systems and their accompanying Operator Structures which took place at the Lorentz Center in Leiden, The Netherlands, on July 21-25, 2008. These papers offer a panorama of selfadjoint and non-selfadjoint operator algebras associated with both noncommutative and commutative (topological) dynamical systems and related subjects. Papers on general theory, as well as more specialized ones on symbolic dynamics and complex dynamical systems, are included.