In this dissertation, we investigate the ways in which search techniques, and in particular metaheuristic search techniques, can be used in cryptology. We address the design of simple cryptographic components (Boolean functions), before moving on to more complex entities (S-boxes). The emphasis then shifts from the construction of cryptographic artefacts to the related area of cryptanalysis, in which we first derive non-linear approximations to S-boxes more powerful than the existing linear approximations, and then exploit these in cryptanalytic attacks against the ciphers DES and Serpent.