To study CO2 capture potential, n-methyl diethanolamine (MDEA) was used to prepare three types of transition-temperature mixtures (TTMs) by mixing methyltriphenylphosphonium bromide (MTPPB) as a hydrogen bond acceptor (HBA) and MDEA as a hydrogen bond donor (HBD) in molar ratios of 1:7, 1:10 and 1:16 HBA to HBD. Fourier transform infrared spectroscopy (FT-IR) results showed that TTMs have almost similar spectra to their HBD (MDEA) with different levels of transmittance and exhibit similar behavior. From the experimental results, it was found that the thermal stability, viscosity and surface tension of TTMs decreased as the concentration of MDEA in the mixture increased. According to response surface methodology (RSM) models and analysis of variance (ANOVA), temperature and molar ratio had a great effect on the viscosity and surface tension of TTMs. The final part of this research was the measurement of CO2 solubility in TTMs at 303.15 K at pressure up to 1.35 MPa. It was found that CO2 solubility in TTMs was enhanced as the MDEA quantity increased in the mixture up to 1:10 mole ratio. However, by increasing MDEA concentration to 16:1 mole ratio, there was a decreasing trend in the CO2 solubility data. Also, all TTMs, particularly TTM containing 10:1 mole MDEA (MTPPB-MDEA 1:10) exhibited an equilibrium loading capacity approaching 1 mole CO2 per mole solvent at high pressure, revealing