An enhancement of the electrical performance of the InAlN/GaN high electron mobility transistors (HEMTs) is demonstrated by the incorporation of post bis(trifluoromethane) sulfonamide (TFSI) treatment. The surface treatment of TFSI solution results in the increase of 2DEG electron mobility from 1180 to 1500 cm2/Vs and thus a reduction of on-state resistance and an increase in transconductance. The results indicate that the positive charge of H+ will decrease the polarization charges of the InAlN barrier under the access region due to the converse piezoelectric effect, leading to the reduced polarization Coulomb field (PCF) scattering in InAlN/GaN HEMT. This offers a possible way to improve the electron mobility and device performance of InAlN/GaN HEMTs for further application.