combinations of metal clusters and organic linkers endow MOFs with controllable physical and chemical properties. [4][5][6][7] Over the last two decades, thousands of MOFs have been prepared and widely applied in many different fields, such as catalysis, [8,9] drug delivery, [10,11] gas separation and storage, [12][13][14][15] and biomedical imaging [16,17] due to these unique properties. Interestingly, MOFs can be purposefully functionalized with chemical groups through in situ synthesis or post-synthetic modification for some special applications without changing their structure. [18][19][20] Besides, much effort has been devoted to developing composite materials integrating MOFs crystals with polymer to further widen their application. [21,22] Triboelectric nanogenerator (TENG) as an eco-friendly energy-harvesting device can effectively convert ambient mechanical energy including wind, human activities, and water flow into electrical energy. [23][24][25][26][27] The nature of the triboelectric pair materials, especially triboelectric polarity, plays an essential role in the triboelectric behaviors of TENG. As far now, most of the triboelectric materials used to assemble the TENG come from the triboelectric series which consists of a few metal and limited polymer. [28] Polydimethylsiloxane (PDMS) is considered one of the broadest parent materials for TENG based on composite by virtue of its unique properties of transparency, high gain-electrons ability, flexibility, and easy fabrication. The surface morphology control with micro/nanostructures and surface functionalization with some appropriate functional groups can improve the output performance. [29][30][31] Zhang et al. reported a common technique to improve the energy density of TENG through a fluorocarbon plasma surface treatment. [29] Besides, adding the filler to the polymer has become a common strategy to optimize the triboelectric behaviors. [32] Most of the materials acting as fillers to fabricate composites are inorganic materials, such as graphene, [33] MXene, [34] and SrTiO 3 . [35] Recently, a few MOFs have been used in triboelectric nanogenerators (TENG) as active fillers. [36][37][38] Our groups reported humidity-resistant PDMS@HKUST-1 TENG and the performance of nanocomposite TENG is not decreased when the relative humidity is increased. [36] Chen et al. reported that planarly aligning 2D MOFs nanoflakes are more excellent for improving the triboelectric behaviors of triboelectric nanogenerators than Metal-organic frameworks (MOFs) are recently used in triboelectric nanogenerator (TENG) to enhance output performance. Although functional groups tremendously influence the output performance of TENG, the effect of functional groups for MOFs on the output performance is yet not systematically studied. In this paper, polydimethylsiloxane (PDMS) composite TENG is designed based on isostructural UiO-66-R (R = H, NH 2 , NO 2 , and Br) family filler, and the effect of filler with various functional groups on the output performance of the TENG is fir...