Attitude dynamics is the theoretical basis of attitude control of spacecrafts in aerospace engineering. With the development of nonlinear dynamics, chaos in spacecraft attitude dynamics has drawn great attention since the 1990s. The problem of the predictability and controllability of the chaotic attitude motion of a spacecraft has a practical significance in astronautic science. This book aims to summarize basic concepts, main approaches, and recent progress in this area. It focuses on the research work of the author and other Chinese scientists in this field, providing new methods and viewpoints in the investigation of spacecraft attitude motion, as well as new mathematical models, with definite engineering backgrounds, for further analysis. Professor Yanzhu Liu was the Director of the Institute of Engineering Mechanics, Shanghai Jiao Tong University, China. Dr. Liqun Chen is a Professor at the Department of Mechanics, Shanghai University, China.