Conventionally, neutralizers in ion thruster systems do not generate thrust force. Hence, the power consumption of a neutralizer negatively affects the thrust efficiency of the ion thruster system. Therefore, in this paper, a negative ion source that generates thrust force as well as neutralizes the positive ion beam was newly developed using fullerene as a propellant so as to realize a more efficient ion thruster system. To develop the negative ion source, two measurements were conducted. The first measurement was an E × B probe to identify the species of positive and negative ions. The second measurement was a magnetically filtered Faraday probe to measure quantitatively the negative ion currents. Based on the measurements, it is concluded that the negative current is not carried by electrons but by negatively charged fullerenes. Finally, the negative ion source was successfully coupled with a positive ion source. To the best of our knowledge, this is the first paper to report the demonstration of an ion thruster using a negative ion source instead of a cathode.