The transition to renewable electricity sources and green feedstock implies the development of electricity storage and conversion systems to both stabilise the electricity grid and provide electrolytic hydrogen. We have recently introduced the concept of a hybrid Ni/Fe battery-electrolyser (battolyser) for this application1. The hydrogen produced during the Ni/Fe cell charge and continued electrolysis can serve as chemical feedstock and a fuel for long-term storage, while the hybrid battery electrodes provide short term storage. Here, we present Ni-Fe layered double hydroxides (NiFe-LDHs) for enhancing the positive electrode performance. The modified Ni(OH)2 material capacity, high rate performance and stability have been tested over a large range of charge rates (from 0.1C to 20C) over 1000 cycles. The Ni-Fe layered double hydroxides allow the capacity per nickel atom to be multiplied by 1.8 in comparison to the conventional β-Ni(OH)2 material which suggests that the nickel content can be reduced by 45% for the same capacity. This reduction of the nickel content is extremely important as this presents the most costly resource. In addition, Fe doped Ni(OH)2 shows improved ionic and electronic conductivity, OER catalytic activity outperforming the benchmark (Ir/C) catalyst, and long term cycling stability. The implementation of this Fe doped Ni(OH)2 material in the Ni/Fe hybrid battery-electrolyser will bring both electrolysis and battery function forward at reduced material cost and energy loss.