With the increase in practical interest in flexible thermoelectric (TE) generators, the demand for high-performance alternatives to brittle TE materials is growing. Herein, we have demonstrated wet-spun CNT fibers with high TE performance by systematically controlling the longitudinal carrier mobility without a significant change in the carrier concentration. The carrier mobility optimized by CNT alignment increases the electrical conductivity without decreasing the thermopower, thus improving the power factor. On further adjusting the charge carriers via mild annealing, the CNT fibers exhibit a high power factor of 432 μW m-1 K-2. Based on the excellent TE performance and shape advantages for modular design of the CNT fiber, the all-carbon based flexible TE generator without an additional metal electrode has been fabricated. The flexible TE generator based on 40 pairs of p- and n-type CNT fibers shows the maximum power density of 15.4 and 259 μW g-1 at temperature differences (ΔT) of 5 and 20 K, respectively, currently one of the highest values reported for TE generators based on flexible materials. The strategy proposed here can improve the performance of flexible TE fibers by optimizing the carrier mobility without a change in the carrier concentration, and shows great potential for flexible TE generators.