As phenol possesses a threat to human health, there is a great demand to search for fast and efficient methods for it to be discharged. In this study, a novel biomaterial was prepared by the immobilization of bacteria on a cationic straw carrier, and the remediation ability of the biomaterial on phenol-containing wastewater was investigated. The free bacteria could degrade 1,000 mg/L phenol within 240 h, while the prepared biomaterial was 192 h, shortening by 48 h that of free bacteria. In addition, the degradation tolerance of biomaterial increased from 1,000 mg/L to 1,200 mg/L than the free bacteria, within 216 h, which shortened by 24 h the degradation time of 1,000 mg/L phenol by free bacteria (240 h). Further, under different pH conditions, the degradation efficiency of phenol by prepared biomaterial was much higher than that of free bacteria. Especially for the lower pH 5, the degradation efficiency of biomaterial was nearly twice that of the free bacteria. This investigation demonstrates that this biomaterial has great potential in the field of remediation of organic pollution.