energy, including solar energy, wind energy, water energy, and bioenergy. Triboelectric nanogenerator (TENG), based on contact electrification and electrostatic induction, was emerging in 2012, [1] which has arisen enormous interest in recent years owing to its ability to harvest energy and convert the energy to electrical energy from human everyday activities, [2,3] the environment of nature, [4][5][6] and similar mechanical motions. TENG shows a wide range of potential applications, such as identified keyboard, [7] sensor power for monitoring driver behavior, [8] smart seat as signal generator, [9] or even the power source for implantable devices, [10] and wearable electronics. [11] Among various kinds of triboelectric materials, poly(dimethylsiloxane) (PDMS) is a kind of ideal negative friction layer candidate due to its high electronegativity, good transparency, and flexibility. [12] Although there are so many advantages of PDMS, there is still a long way to improve the output characteristics of PDMS-based TENG, which can better satisfy the energy needs of various devices in the future. Many researchers have proposed diverse methods such as increasing actual triboelectric area by the preparation of surface micro-nanostructures using photolithography templates, [13][14][15] and surface physical/chemical treatments. [14,16] Unfortunately, these methods often require complicated processes or delicate instruments. In addition, dielectric materials [17,18] or conductive materials [19,20] can be doped in PDMS to build micro-capacitance structures to improve output characteristics. However, these often deteriorate the transparency and flexibility of TENG. Although the PTFE material has attracted much attention due to high electronegativity for TENG applications, [21][22][23][24][25][26][27] its transparence is still far from satisfactory. Here it should be noted that the integration of flexible and transparent characteristics has attracted much attention, and various kinds of novel optoelectronic and electronic devices have been developed in recent years, including artificial skins, [28,29] various sensors, [30,31] and transistors. [32,33] In this study, one simple and low-cost method was demonstrated to modify the PDMS film as the negative friction layer of TENG without degrading its transparency and flexibility, and meanwhile the output performance was obviously improved.