We present the development of a low-frequency nonthermal plasma-jet system, where the surrounding-gas condition of the plasma jet is precisely controlled in open air. By restricting the mixing of the ambient air into the plasma jet, the plasma jet can be selectively changed from a N2 main discharge to an O2 main discharge even in open air. In the plasma-jet system with the controlled surrounding gas, the production of reactive oxygen and nitrogen species is successfully controlled in deionized water: the concentration ratio of NO2
− to H2O2 is tuned from 0 to 0.18, and a high NO2
− concentration ratio is obtained at a N2 gas ratio of 0.80 relative to the total N2/O2 gas mixture in the main discharge gas. We also find that the NO2
− concentration is much higher in the plasma-activated medium than in the plasma-activated deionized water, which is mainly explained by the contribution of amino acids to NO2
− generation in the medium.