Both high energy density and high power density are vitally required for new applications such as electric vehicles. Here we present a comparison of two well-crystallised layered double hydroxides, [Ni4Al(OH)10]OH and [Ni4Al(OH)10]NO3, which shows that the former can maintain a better discharge capacity, 294–299mAhg−1, than the latter, 233–287mAhg−1 at a current density of 2000mAg−1 within about 300 cycles, although both electrodes deliver a similar capacity of 326mAhg−1 at 200mAg−1 initially. It is believed that both the more watery interlayer space in [Ni4Al(OH)10]OH than in [Ni4Al(OH)10]NO3 and the morphologic changes induced by anion exchange of NO3 − by OH− during electrochemical cycles play key roles in their behaviour.