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As the essential element of a triboelectric nanogenerator (TENG), friction layers play key roles that determine the device performance, which can be enhanced by material selection and surface modification. In this work, we have embedded aligned carbon nanotubes (CNTs) on the polydimethylsiloxane (PDMS) surface as the effective dielectric layer to donate electrons. This layer not only increases the electron generation for the output, but also shows notable stretchability. The length and the properties of the aligned CNTs can be controlled precisely. Using the 40 μm CNT as an example, the fabricated CNT–PDMS TENG shows an output voltage of 150 V and a current density of 60 mA m−2, which are 250% and 300% enhancement compared to the TENG using directly doped PDMS/multiwall carbon nanotubes, respectively. The maximum power density of this TENG reaches 4.62 W m−2 at an external load of 30 …