Hybrid organic-inorganic layered double hydroxide materials have been prepared with an ultra-high aspect ratio via an environmentally friendly co-hydration approach where metal hydroxides and adamantane-carboxylic acid were used as the reagents. The method avoids use of either acidic or basic precipitation methods, or using a large excess of anion. The effect of organic anion, metal cation and synthesis method on developing ultra-high aspect ratio crystallites was studied.