Models of phase oscillators have proven to be a very convenient tool to investigate the emergence of dynamical order in complex systems, and their use has been spreading across disciplines ranging from chemistry to biology, neurology and economics, to name a few. In particular, they have been used as a probing model to study the interplay between network structure and dynamics on networks for systems of broadly different nature. This work concerns itself with the emergence and destruction of dynamical order in networks of phase oscillators. Particular attention is payed to the implementation of methods to control the formation and behavior of self-organized dynamical patterns in the transition landscape between synchronization and chaos. This book consists of a revised version of the author's doctoral thesis, presented at the Technische Universitat Berlin in January 2010, and defended with a magna cum laude distinction."