Computational intelligence (CI) has attracted the attention of many researchers for its effectiveness in solving different kinds of problems. It has been applied to solve problems in a wide area of applications. The aim of this chapter is to present an overview of existing literature about the applications of CI in cryptology. It demonstrates and studies the applicability of CI in cryptology. The problems examined in this chapter are the automated design of cipher systems, and the automated cryptanalysis of cipher systems. It has been shown that CI methods, such as genetic algorithms, genetic programming, Tabu search, and memetic computing are effective tools to solve most of cryptology problems.