Electrospun polyamide (PA) 66 nanofiber bundles with high conductivity, improved strength, and robust flexibility were successfully manufactured through simply adsorbing multiwall carbon nanotubes (MWNTs) on the surface of electrospun PA66 nanofibers. The highest electrical conductivity (0.2 S/cm) and tensile strength (103.3 MPa) were achieved for the bundles immersed in the suspension with 0.05 wt % MWNTs, indicating the formation of conductive network from adsorbed MWNTs on the surface of PA66 nanofibers. The decrease of porosity for the bundles immersed in the MWNT dispersion and the formation of hydrogen bond between PA66 nanofibers and MWNTs suggest a superb interfacial interaction, which is responsible for the excellent mechanical properties of the nanocomposite bundles. Furthermore, the resistance fluctuation under bending is less than 3.6%, indicating a high flexibility of the nanocomposite bundles. The resistance of the nanocomposite bundle had a better linear dependence on the temperature applied between 30 and 150 °C. More importantly, such highest working temperature of 150 °C far exceeded that of other polymer-based temperature sensors previously reported. This suggests that such prepared MWNTs-adsorbed electrospun PA66 nanofiber bundles have great potentials in high temperature detectors.