Microalgae biofilm-based culture has attracted much interest due to its high harvest efficiency and low energy requirements. Using light-emitting diodes (LEDs) as light source for microalgae culture has been considered as a promising choice to enhance the economic feasibility of microalgae-based commodities. In this work, the LED power conversion capability and CO2 fixation rate of microalgae biofilms (Chlorella ellipsoidea and Chlorella pyrenoidosa) cultured under different light spectra (white, blue, green and red) were studied. The results indicated that the power-to-biomass conversion capabilities of these two microalgae biofilms cultured under blue and white LEDs were much higher than those under green and red LEDs (C. ellipsoidea: 32%–33% higher, C. pyrenoidosa: 34%–46% higher), and their power-to-lipid conversion capabilities cultured under blue LEDs were 61%–66% higher than those under green LEDs. The CO2 fixation rates of these two biofilms cultured under blue LEDs were 13% and 31% higher, respectively, than those under green LEDs. The results of this study have important implications for selecting the optimal energy-efficient LEDs using in microalgae biofilm-based culture systems.