The present study aimed to determine the effects of multi-walled carbon nanotubes (MWCNTs) concentrations (0, 0.1, 1, 5, 10 mg·L− 1) on tetracycline (TC) and biogas slurry nutrients removal by microalgae Chlorella vulgaris cultivation. Treatments with 1 mg·L− 1 MWCNTs yielded maximum dry weight and cells quantity of 0.81 ± 0.008 g·L− 1 and 5.83×107 cell·L− 1, respectively. The results of chlorophyll a were consistent with rapid fluorescence induction kinetics (OJIP-test), indicating that moderate MWCNTs concentration could enhance microalgal photosynthesis. Maximum chemical oxygen demand (COD), total phosphorus (TP), total nitrogen (TN), tetracycline (TC), and CO2 removal efficiencies were 90.43 ± 5.15%, 78.12 ± 4.33%, 77.07 ± 4.12%, 89.64 ± 3.08%, and 64.26 ± 0.71%, respectively when treated with 1 mg·L− 1 MWCNTs. Of the five MWCNTs concentrations set in this study, the optimal concentration was 1 mg·L− 1 for nutrient and CO2 removal efficiencies. These results indicated that moderate MWCNTs concentrations would promote tetracycline and nutrients removal by enhancing Chlorella vulgaris photosynthesis activity.