“…Triboelectric nanogenerators (TENGs) are promising energy harvesters that have attracted great attention in recent decades owing to their advantages, such as high output voltage, simple fabrication, low cost, and autonomy in material selection. − However, increasing the practicability of TENGs relies on further enhancements in their performance, notably in parameters such as output performance and sustainability. − Generally, the output performance of TENGs is heavily dependent on the triboelectric charge generation and charge separation processes. − Several strategies have been developed to improve charge generation and separation, such as triboelectric material development, device structure optimization, ionized air injection, and micro/nanoscale surface modification. − From the viewpoint of the materials, the dielectric properties and the work functions of the two materials in contact are vital points. ,− However, polymers, the most widely used negative triboelectric materials, possess intrinsically low dielectric constants, limiting the output performances of TENGs. − To overcome this long-standing issue, extensive research has been conducted to enhance the output performance of TENG devices by developing composites that physically integrate inorganic particles with a high dielectric constant into a polymer matrix. − However, the high surface energy of inorganic particles causes their aggregation and phase separation from the polymer matrix, inevitably leading to a high dielectric loss and low breakdown strength. , Although core–shell hybrids chemically incorporating polymer shells into the surface of inorganic cores have recently emerged as a promising alternative, they still suffer from insufficient dispersibility and film uniformity, unfortunately remaining limited in solving the challenge of the aforementioned deteriorated electrical properties in energy harvesting and storage applications, including TENGs. …”