Non-thermal plasma driven ammonia synthesis has great potential for future industrial applications due to its low theoretical energy requirements. To achieve technological advancement and environmental sustainability, it is crucial to boost the energy yield in plasma-assisted ammonia synthesis. Therefore, optimizing energy transfer and utilization are key strategies for enhancing energy efficiency. In this study, dielectric barrier discharge driven by a nanosecond pulsed power supply is used to enhance plasma-assisted ammonia synthesis by controlling the energy transfer through the addition of noble gases. It was found that the addition of noble gases changed the plasma characteristics, significantly improved the uniformity of the discharge, and achieved a high energy yield for ammonia synthesis. The effects of additive amounts of argon (Ar) and helium (He), as well as the pulse parameters including the pulse voltage, pulse repetition frequency, pulse width, and pulse rise time on the energy yield of ammonia synthesis are discussed. The inclusion of noble gases expanded the pathway for gas-phase reactions, with the active components of critical reactions examined through optical emission spectra. This analysis revealed an increased presence of both N2+ and N2* particles in the reaction’s rate-limiting step, attributed to the addition of noble gases. Finally, a zero-dimensional (0D) plasma chemical kinetic model was established to investigate the influence of Ar addition on the reaction mechanism of ammonia synthesis.