The chapter introduces developments in intelligent optimal control systems and their applications in structural engineering. It provides a good background on the subject starting with the shortcomings of conventional vibration control techniques and the need for intelligent control systems. Description of a few basic tools required for intelligent control such as evolutionary algorithms, fuzzy rule base, and so forth, is outlined. Examples on vibration control of benchmark building and bridge under seismic excitation are presented to provide better insight on the subject. The chapter provides necessary background for a reader to work in intelligent structural control systems with real-life examples. Current trends in the research area are given and challenges put forward for further research.