Bioaugmentation is a promising technology for pollutant elimination from stressed environments, and it would provide an efficient way to solve challenges in traditional biotreatment of wastewater with high strength of ammonia nitrogen (NH4+-N). A high NH4+-N-resistant bacteria strain, identified as Bacillus cereus (Jlu BC), was domesticated and isolated from the bacteria consortium in landfill leachate. Jlu BC could survive in 100 g/L NH4+-N environment, which indicated its extremely high NH4+-N tolerance than the stains found before. Jlu BC was employed in the bioaugmented system to remove high strength of NH4+-N from landfill leachate, and to increase the removal efficiency, response surface methodology (RSM) was used for optimizing bioaugmentation degradation conditions. At the optimum condition (initial pH 7.33, 4.14 days, initial chemical oxygen demand [COD] concentration [18,000 mg/L], 3.5 mL inoculated domesticated bacteria strain, 0.3 mg/mL phosphorus supplement, 30 °C, and 170 rpm), 94.74 ± 3.8% removal rate of NH4+-N was obtained, and the experiment data corresponded well with the predicted removal rate of the RSM models (95.50%). Furthermore, COD removal rate of 81.94 ± 1.4% was obtained simultaneously. The results presented are promising, and the screened strain would be of great practical importance in mature landfill leachate and other NH4+-N enrichment wastewater pollution control.