Four-probe resistivity measurements were performed on the TMTTeN crystal by using a diamond anvil high-pressure cell up to 30 GPa. The crystal could not be metallized though the room-temperature resistivity decreased to a very small value (1.5 x 10(-3) Omega cm). Although single-component molecular metals are composed of molecules, the pressure-induced metallization of a single-component pi molecular crystal while maintaining the initial molecular structure appears to be very difficult.