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Supporting Information Transparent and Self-supporting Graphene Films with Wrinkled- Graphene-Wall-assembled Opening Polyhedron Building Blocks for High Performance Flexible/Transparent Supercapacitors Na Li,, Xuankai Huang, Haiyan Zhang, Yunyong Li, Chengxin Wang, School of Material and Energy, Guangdong University of Technology, Guangzhou, 510006, P. R. China State key laboratory of optoelectronic materials and technologies, School of Material Science and Engineering, Sun Yat-sen (Zhongshan) University, Guangzhou 510275, People s Republic of China * Correspondence and requests for materials should be addressed to N.L. e-mail: lina150907@gdut.edu.cn and C.X.W. e-mail: wchengx@mail.sysu.edu.cn S-1

Figure S1: SEM micrograph of a curved STF-GF with a smooth deflection edge due to the deforming opened-hollow polyhedron building units. 3µm S-2

Figure S2: High-resolution TEM micrographs of the wrinkled graphene wall like a hairy carpet, thus enlarging the efficient surface area of the STF-GF. 500 nm S-3

Figure S3: SEM micrographs of STF-GF before and after being treated with concentrated H 2 SO 4 /HNO 3. Before After 5 5 Figure S4: Raman spectrum of STF-GF before and after being treated with concentrated H 2 SO 4 /HNO 3. After treatment Before 2D D G D' 1500 2500 3000 Raman Shift (cm -1 ) S-4

Figure S5: Ragone plot of the device calculated based on STF-GF/electrolyte and the total device. The volumetric energies as a function of power density are compared with previously reported flexible transparent supercapacitors. Energy density (Wh cm -3 ) 10-2 10-3 10-4 10-5 STF-GF-based sample/electrolyte R R 30 38 R R 15 R 23 14 R 37 R 15 10-6 10-4 10-3 10-2 10-1 10 0 10 1 10 2 R 39 STF-GF-based Total Device Average power density (W cm -3 ) S-5

Table S1: Comparison results among transparent/nontransparent supercapacitors. Material Transmittance,flexibility Specific capacitance Energy density Power density Ref. MWCNT film Transparent/flexible (62%) 146µF/cm2(based on electrode) 12.5Wh/Kg(based on electrode) 13.9KW/Kg (based on electrode materials) 1 PANI&MWCNT Transparent/flexible(60%) 300F/g (based on electrode) 2 MWCNT film Transparent/flexible (75%) 7.3F/g (for device) 2.4Wh/Kg (based on electrode) 0.9Kw/Kg (based on electrode) 3 PANI&SWCNT Transparent/flexible (55%) 55F/g (for device) 4 nano-energied carbon films Transparent/flexible (71%) 409µF/cm2 (for device) 47µWh/cm3 (for electrolyte/material) 19mW/cm 3 (based on electrolyte /) 5 grpahene film Transparent/flexible (67%) 12.4µF/cm2 (for device) 2.94Wh/Kg (based on electrode) 438.6KW/Kg (based on electrode) 6 CVD graphene Transparent/stretchable (50-60%) 5.8µF/cm2 (7.6F/g) 7 CVD graphene Transparent/flexible 80.7µF/cm2 (for device) 2.5 mwh/cm3(for device) 495W/cm 3 (for device) 8 CVD grapehene Transparent/flexible 80µF/cm2 (for device) 9 RGO film Transparent/flexible 394µF/cm2 (for device)s 9 CVD graphene Transparent/stretchable 4.27µF/cm2 (for device) 0.20 nwh/ cm2 36.48 µw/cm 2 10 FFT-GP Transparent/flexible (electrode79%) 3.3mF/cm 2 (for device) 430µWh/cm 3 (for electrolyte/material) 190mW/cm 3 (for electrolyte/materials) 11 SFT-GF Transparent/flexible (device 51.6%) 4.21 mf/cm 2 (for device) 552.3 Wh/cm 3 561.9 mw/cm 3 Here onion-likecarbon Nontransparent/flexible 1.7mF/cm 2 (for device) 10 mwh/cm 3 (for device) 1Kw/cm 3 (for device) 12 Fe 2O 3//MnO 2 Nontransparent/flexible 1.5F/cm 3 0.55 mwh/cm 3 (for device) 150 mw/cm 3 (for device) 13 NPG-PPy//NPG-PPy Nontransparent/flexible 30 F/cm 3 2.8 mwh/cm 3 (for device) 56.7 W/cm 3 (for device) 14 MnO2//carbon fiber Nontransparent/flexible 10 F/cm 3 5 mwh/cm 3 (for device) 929 mw/cm 3 15 WO 3@MoO 3//PANI Nontransparent/flexible 216mF/cm 2 1.9 mwh/cm 3 (for device) 730 mw/cm 3 16 S-6

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