The concept of tuning phenomenon in binary hydrate systems has been suggested to enhance the gas storage capacity through molecular interactions. In this report, the existence of critical guest concentration (CGC) is investigated by means of spectroscopic methods. The existence of the critical guest concentration can act as a limiting factor in the application areas of binary hydrates. Therefore, it should be taken into account before applying this concept to application fields. In addition, further research on this concept using other hydrate systems is required to clarify the present findings.