The synthesis of layered cobalt hydroxides featuring triangular ordering, and the exploration of their phase conversion chemistry, is the main focus of this thesis. An introduction to cobalt hydroxide chemistry and to structurally similar compounds, with an emphasis on layered metal hydroxides, is given in Chapter 1. Novel synthetic methods, structural analysis and the most recent development for layered double hydroxides are sequentially introduced. The aim of the thesis is followed up as an extension of the existing work.