Surface hardening of commercially pure titanium using bipolar pulsed nanocrystalline plasma electrolytic carbonitriding has been studied in this investigation. The coating process has been performed on triethanolamine-based electrolytes using a cooling bath. The nanostructure of obtained compound layers was examined with figure analysis of SEM nanographs. The effects of process variables (i.e., frequency, temperature of electrolytes, applied voltage, and treatment time) have been studied experimentally. Statistical methods were used to achieve the optimum size of nanocrystals. Finally, the contribution percentage of the effective factors of pulsed current was revealed, and confirmation showed the validity of obtained results. It has also been revealed that by changing the size of nanocrystalline carbonitrides, other properties of the coating will change significantly.