A major limiting factor in the development of algae as a feedstock for the bioenergy industry is the consistent production and supply of biomass. This study is the first to access the suitability of the freshwater macroalgal genus Oedogonium to supply biomass for bioenergy applications. Specifically, we quantified the effect of CO2 supplementation on the rate of biomass production, carbon capture, and feedstock quality of Oedogonium when cultured in large-scale outdoor tanks. Oedogonium cultures maintained at a pH of 7.5 through the addition of CO2 resulted in biomass productivities of 8.33 (0.51) g DW m2 day1 , which was 2.5 times higher than controls which had an average productivity of 3.37 (0.75) g DW m2 day1 . Under these productivities, Oedogonium had a carbon content of 41–45% and a higher heating value of 18.5 MJ kg1 , making it an ideal biomass energy feedstock. The rate of carbon fixation was 1380 g C m2 yr1 and 1073.1 g C m2 yr1 for cultures maintained at a pH of 7.5 and 8.5, and 481 g C m2 yr1 for cultures not supplemented with CO2. This study highlights the potential of integrating the large-scale culture of freshwater macroalgae with existing carbon waste streams, for example coal-fired power stations, both as a tool for carbon sequestration and as an enhanced and sustainable source of bioenergy.