The effects of five different microalgae-fungi on nutrient removal and CO2 removal were investigated under three different CO2 contents (35%, 45% and 55%). The results showed that the highest nutrient and CO2 removal efficiency were found at 55% CO2 by cocultivation of different microalgae and fungi. The effect of different initial CO2 concentration on the removal of CO2 from microalgae was significant, and the order of CO2 removal efficiency was 55% (v/v) >45% (v/v) >35% (v/v). The best nutrient removal and biogas purification could be achieved by co-cultivation of C. vulgaris and G. lucidum with 55% initial CO2 content. The maximum mean COD, TN, TP and CO2 removal efficiency can reach 68.29%, 61.75%, 64.21% and 64.68%, respectively under this condition. All highest COD, TN, TP and CO2 removal efficiency were more than 85%. The analysis of energy consumption economic efficiency revealed that this strategy resulted in the highest economic efficiency. The results of this work can promote simultaneously biological purification of wastewater and biogas using microalgal-fungal symbiosis.