A simultaneous nitrification and denitrification (SND) bioaugmention system with Pseudomonas sp. HJ3 inoculated was established to explore the potential of simultaneous phenol and nitrogen removal in coal gasification wastewater (CGW). When the concentration of influent chemical oxygen demand (COD) and total phenols (TPh) was 1,765.94 ± 27.43 mg/L and 289.55 ± 10.32 mg/L, the average removal efficiency of COD and TPh at the stable operating stage reached 64.07% ± 0.76% and 74.91% ± 0.33%, respectively. Meanwhile, the average removal efficiency of NH4 +-N and total nitrogen (TN) reached 67.96% ± 0.17% and 57.95% ± 0.12%, respectively. The maximum SND efficiency reached 83.51%. Furthermore, SND bioaugmentation performed with good nitrification tolerance of phenol shock load and significantly reduced toxic inhibition of organisms. Additionally, the microbial community analysis indicated that Pseudomonas sp. HJ3 was the predominant bacterium in the SND bioaugmentation system. Moreover, the indigenous nitrogen removal bacteria such as Thauera, Acidovorax and Stenotrophomonas were enriched, which further enhanced the nitrogen removal in the SND bioaugmentation system. The results demonstrated the promising application of SND bioaugmentation for enhancing simultaneous phenol and nitrogen removal in CGW treatment.