The dataset contains results from application of a mid-infrared frequency comb-based Fourier transform spectrometer to measure high-resolution spectra of plasmas containing hydrogen, nitrogen, and a carbon source in the 2800 – 3400 cm–1 range. The spectrally broadband and high-resolution capabilities of this technique enable quantum-state-resolved spectroscopy of multiple plasma-generated species simultaneously, including CH4, C2H2, C2H6, NH3, and HCN, providing detailed information beyond the limitations of current methods. Using a line-by-line fitting approach, we analyzed 548 resolved transitions across five vibrational bands of plasma-generated HCN. The results indicate a significant non-thermal distribution of the populations among the quantum states, with distinct temperatures observed for lower and higher rotational quantum numbers, with a temperature difference of about 62 K. Broadband state-resolved-spectroscopy via comb-based methods provides unprecedented fundamental insights into the non-thermal nature of molecular plasmas – a detailed picture that has never been accomplished before for such complex non-thermal environment.