Various means have been proposed to solve problems such as high ash content and complex composition in the recycling of nickel-containing residue produced by battery manufacturing enterprises. Microwave roasting pretreatment is proposed to improve the nickel leaching rate from the residue. The effect of different experimental conditions like microwave roasting temperatures, roasting times, and microwave powers on the nickel leaching rate was studied. It was found that the effect of roasting temperature on the nickel leaching rate was more significant than those of roasting time and microwave power. Meanwhile, after microwave roasting pretreatment, the rate of nickel leaching from the residue could be increased by 20.43%, and weight of the material could also be reduced by more than 21%. After microwave roasting at 450°C, there was no significant change in the main phases of the material, but the surface of the particles exhibited an apparent stratified dissociation phenomenon. Response surface methodology (RSM) was used to optimize the parameters of microwave roasting with nickel leaching rate as the response value. The results showed that the nickel leaching rate could reach 93.11% for roasting at the microwave power of 962 W for 6.2 min under the temperature of 452°C.