As a new energy harvesting invention [4] with great potential application value, [5] triboelectric nanogenerator (TENG) has gradually advanced, [6] whether in theoretical research, structural innovation, or application development, since its discovery in 2012, [7] which has four main applications nowadays: micronanoenergy, [8] self-powered sensor, [9] blue energy, [10] and high-voltage application. [11] Different from the low-voltage characteristic of the electromagnetic generator, TENG can be considered as a current source [12] with high voltage and low current output characteristics. Therefore, the research on the high-voltage application scenarios and mechanism of TENGs is gradually receiving extensive attention from researchers. [13] Lin et al. designed a TENG with a radially distributed disk structure for the first time, which opens up many novel structures and potential applications. [14] Then, a freestanding rotary triboelectric nanogenerator (FR-TENG) with radial arrays of microsized sectors was designed, which achieved multiple charge transfer and generated higher short-circuit current (I SC ). [15] FR-TENG has received widespread attention due to its characteristics of higher open-circuit voltage (V OC ) and shortcircuit current. [16] However, since the conventional FR-TENGThe soft-contact freestanding rotary triboelectric nanogenerator (FR-TENG), with the capabilities of high output performance and excellent efficiency, presents interesting applications in driven nonequilibrium plasma jets, mass spectrometry, electrospinning, and so on. For enhancing the output performance of FR-TENG, detailed and in-depth research focusing on the design method is discussed in this paper, mainly consisting of the following four parts: 1) design reasonable geometric structure, 2) select triboelectric layers, 3) choose a reasonable signal acquisition, and 4) investigate influencing factors. Benefiting from this four-step systematic research, a modified FR-TENG with better output performance is successfully constructed. A corresponding open-circuit voltage density of 1.27 × 10 5 V m −2 is achieved, which is over twofold higher compared to the largest one among the previous similar articles. Therefore, the four-step systematic research is demonstrated to remarkably enhance the output performance of the soft-contact FR-TENG. This work not only presents a modified FR-TENG with ultrahigh voltage density that inhibits bacterial corrosion, enables high-voltage electrostatic dust removal, and enables impressive current cathodic protection of marine pipelines and urban buried pipelines, but also can be regarded as guidance for the design of soft-contact FR-TENG.