Nickel–cobalt oxyhydroxide has been delaminated by tetrabutylammonium (TBA+) intercalation in aqueous media. The electrochemical performance of the different materials obtained during delamination has been evaluated, with special emphasis on the effect of the intercalated species and their influence on the behavior of the delaminated material, toward electrochemical energy storage applications. Delamination in TBAOH, reported for the first time for nickel–cobalt oxyhydroxide in aqueous media, is an excellent route to increase the number of electrochemically active sites and to enhance the capacity of nickel–cobalt oxyhydroxide. Results show an increase in capacity from 112 mA·h·g–1 in 1 M LiOH at 1 A·g–1 for the nondelaminated precursor to 165 mA·h·g–1 after exfoliation and restacking. Thus, carefully designed exfoliation is a promising route to enhance the performance of electrode materials for electrochemical energy storage.