It is expected that CO2 concentration will increase in the air, thereby stimulating the photosynthesis process and, hence, plant biomass production. In the case of legumes, increased biomass due to higher CO2 concentration can stimulate atmospheric nitrogen (N2) fixation in the nodules. However, N2 fixation is inhibited by external N supply. Thus, biomass production and N2 fixation were analysed in two legumes (Pisum sativum L. and Vicia faba L.) grown at two levels of CO2 and three N levels. P. sativum reduces fixation with high soil N (facultative), while V. faba maintains high fixation regardless of soil N levels (obligate). The N2 fixation and plant and nodule biomass of the two species were evaluated in a pot experiment under controlled conditions using growth chambers with artificial CO2 supply and N addition. The proportion of N derived from the air (%Ndfa) present in the plants’ biomass was calculated from the natural abundance of 15N and the N concentration of plant tissues using nonlegumes reference plants. Additionally, N content data are presented for both species growing at two levels of air CO2. The data may be useful for plant physiologists, especially those working on biological N2 fixation with non-model legumes at elevated CO2.