environmental variations such as isolated places, indoors, and dark surroundings. [1][2][3] The mechanical energy for wearable electronics is more reliable and environmentally independent as well as continuous energy source than the solar or the thermal energy, and it is easily convertible to the electrical energy using electromagnetic induction, [4] triboelectric effect, [5] piezoelectric principle, [6] and so forth. Among them, in particular, triboelectric and/or piezoelectric effect-driven energy devices have drawn much higher attentions for future self-powered electronic system than electromagnetic induction-utilized devices due to simple processes, excellent flexibility, high voltage, and power output as well as easy size-scaling, etc. [5][6][7][8][9][10] Since the output power which can be derived from human motion-related activities mainly depends on the operating frequencies and the degree of deformation (i.e., strain), power generators should be composed of highly flexible and durable materials having robust structures. [6,11,12] Among various flexible substrates, the paper, consisting of multiple cellulose fibers, is identified as the most eco-friendly substrate material with very low cost and excellent recyclability. [12][13][14] Furthermore, the use of paper substrates for flexible devices is potentially beneficial for the Key solutions for material selection, processing, and performance of environmentally friendly high-power generators are addressed. High voltage and high power generation of flexible devices using piezoelectric Bi 0.5 (Na 0.78 K 0.22 ) TiO 3 nanoparticle filler-polydimethylsiloxane (PDMS) elastomeric matrix for a lead-free piezoelectric composite film on a cellulose paper substrate is demonstrated. To elucidate the principle of power generation by the piezoelectric composite configuration, the dielectric and piezoelectric characteristics of the composite film are investigated and the results are compared with those of theoretical modeling. The paper-based composite generator produces a large output voltage of ≈100 V and an average current of ≈20 µA (max. ≈30 µA) through tapping stimulation, which is a record-high performance compared to previously reported flexible lead-free piezoelectric composite energy harvesters. Moreover, a triboelectric-hybridized piezoelectric composite device using a micro-patterned PDMS shows a much higher output voltage of ≈250 V and output power of ≈0.5 mW, which drives 300 light-emitting diodes. These results prove that a new class of paper-based and lead-free energy harvesting device provides a strong possibility for enlarging the functionality and the capability of high-power scavengers in flexible and wearable electronics such as sensors and medical devices.One of the best power sources for the human activity-based self-powered wearable electronic devices is the mechanical energy source because it is easily obtained from biological activities or human motions regardless of the location and the