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We report for the first time to our knowledge large-signal measurements performed at 600 MHz and in time domain on carbon nanotube field-effect transistors (CNFETs) using a large-signal network analyzer. To overcome the very high mismatch between the high CNFET impedance and the basic 50-Omega configuration of the setup, the output impedance was matched with the help of an experimental active load-pull configuration. Hence, we were able to observe under large-signal conditions the nonlinear behavior of CNFETs. Static measurements and continuous-wave S ij -parameter measurements were made for many different biases. They were used in order to determine a nonlinear electrical model that has been validated thanks to the nonlinear measurements. The developed model opens the way for electrical CNFET circuit simulation and nonlinear applications of these devices.