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The extended-gate field-effect transistors (EGFETs) with only the carbon-nanotube (CNT) thin film as both the sensing membrane and the contact electrode have been demonstrated for the first time to exhibit superior pH sensing characteristics. The continuous-wave laser was necessary to improve the pH sensitivity to be 50.9 mV/pH and the linearity values to be 0.9978 for pH = 3 to pH = 13 wide sensing range, respectively. It implied that the laser energy would unzip the chemically modified multiwalled CNTs (MWCNTs) into numerous graphite slices, resulting in the elevated sensing sites and the improved electrical and sensing properties. Therefore, the laser-irradiated MWCNT network is promising for the applications in the flexible and transparent pH-EGFETs.