Figure S4 Cross-section morphology of the resultant paper prepared by poorly dispersed

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1 Supporting Information Highly Thermally Conductive Composite Papers Prepared Based on the Thought of Bioinspired Engineering Yimin Yao,,, Xiaoliang Zeng,,, Rong Sun, *, Jian-Bin Xu, Ching-Ping Wong,, Shenzhen Institutes of Advanced Technology, Chinese Academy of Sciences, Shenzhen, China. Shenzhen College of Advanced Technology, University of Chinese Academy of Sciences, Shenzhen, China. Department of Electronics Engineering, The Chinese University of Hong Kong, Hong Kong, China. School of Materials Science and Engineering, Georgia Institute of Technology, Atlanta, GA 30332, United States. Yimin Yao and Xiaoliang Zeng contributed equally. *Corresponding Author: Rong Sun: Tel Postal address: 1068 Xueyuan Avenue, Shenzhen University Town, Shenzhen, China. Contents: Figure S1. DLS result of BNNS water suspension. Figure S2. Elemental distribution of BNNS Ag hybrids. Figure S3. Elemental distribution of SiCNW Ag hybrids. Figure S4 Cross-section morphology of the resultant paper prepared by poorly dispersed components. Figure S5. (a-f) BNNS Ag hybrids generated in the action system of C BNNS :C AgNO3 =1:1, 2:1, 3:1, 5:1, 10:1, and 15:1, respectively. Figure S6. (a-c) SiCNW Ag hybrids generated in the action system of C SiCNW :C AgNO3=4:1, 8:1, 16:1, respectively. Figure S7. Variation of SiCNW length distribution with ball-milling time. Figure S8. Through-plane conductivities of BNNS/PVA, BNNS Ag/PVA, and BNNS Ag/SiCNW Ag/PVA composite papers. Figure S9. In-plane conductivity vs BNNS content in BNNS/CNF paper. Table S1. Comparison of thermal conductivity of our composite paper with other reported oriented BN-containing composites or films along the orientation. Table S2. Summary of the mechanical properties of the prepared papers by tensile testing. S-1

2 Figure S1. DLS result of BNNS water suspension. S-2

3 Figure S2. Elemental distrubution of BNNS Ag hybrids. S-3

4 Figure S3. Elemental distrubution of SiCNW Ag hybrids. S-4

5 Figure S4. Cross-section morphology of the resultant paper prepared by poorly dispersed components. S-5

6 Figure S5. (a-f) BNNS Ag hybrids generated in the action system of CBNNS:CAgNO3=1:1, 2:1, 3:1, 5:1, 10:1, and 15:1, respectively. S-6

7 Figure S6. (a-c) SiCNW Ag hybrids generated in the action system of C SiCNW :CA gno3 =4:1, 8:1, 16:1, respectively. S-7

8 Figure S7. Variation of SiCNW length distribution with ball-milling time. By statistic evaluation with more than one hundred tubes in SEM images of dispersed SiCNWs, it is revealed that about 30% of SiCNWs are longer than 10 µm, 36% of the SiCNWs are in a length range from 6 to 10 µm, 30% of the SiCNWs are in a length range from 2 to 6 µm, and 18% are shorter than 2 µm after ball-milling for 12 h. With extra ball-milling treatment for 12 h, the percentage of SiCNWs with length distribution longer than 10 µm and between 6 and 10 µm was changed to 17% and 21%, respectively, indicating an obvious shortening effect. When further prolonging the ball-milling treatment time to 36 h, the SiCNWs were massively shortened to less than 6 µm. S-8

9 Figure S8. Through-plane conductivities of BNNS/PVA, BNNS Ag/PVA, and BNNS Ag/SiCNW Ag/PVA composite papers. S-9

10 Figure S9. In-plane conductivity vs BN content in BNNS/CNF paper. S-10

11 Table S1. Comparison of thermal conductivity of our composite paper with other reported oriented BN-containing composites or films along the orientation. In-plane thermal Fillers Matrix Method of orientation Loading conductivity (Wm -1 K -1 ) Year Ref BNNS PVA Mechanical stretching 15 vol% BN PI Spin-casting 60 vol% BN PVB Tape-casting 50 vol% BNNS Silicone rubber Shearing on a two-roll mill 30.8 vol% BNNS Natural rubber Shearing on a two-roll mill 30.8 vol% BN Silicone Magnetically aligning 9.14 vol% BNNS Epoxy Ice-templated assembling 9.29 vol% BN+SiC Epoxy Magnetically aligning 40 vol% BN Epoxy Magnetically aligning 30 vol% BNNS GO Vacuum-assisted filtration 95 vol% BNNS+SiCNW PVA Vacuum-assisted filtration 95 vol% This work S-11

12 Table S2. Summary of the mechanical properties of the prepared composite papers by tensile testing. Samples Tensile strength (MPa) Young s modulus (GPa) Toughness (MJ m -3 ) BNNS/PVA paper 9.8± ± ±0.001 BNNS Ag/PVA paper BNNS Ag/SiCNW Ag/PVA paper 29.9± ± ± ± ± ±0.03 S-12

13 References: 1. Song, W.-L.; Wang, P.; Cao, L.; Anderson, A.; Meziani, M. J.; Farr, A. J.; Sun, Y.-P., Polymer/Boron Nitride Nanocomposite Materials for Superior Thermal Transport Performance. Angew. Chem. Int. Ed. 2012, 51, Tanimoto, M.; Yamagata, T.; Miyata, K.; Ando, S., Anisotropic Thermal Diffusivity of Hexagonal Boron Nitride-Filled Polyimide Films: Effects of Filler Particle Size, Aggregation, Orientation, and Polymer Chain Rigidity. ACS Appl. Mater. Interfaces 2013, 5, Ahn, H. J.; Eoh, Y. J.; Park, S. D.; Kim, E. S., Thermal Conductivity of Polymer Composites with Oriented Boron Nitride. Thermochim. Acta 2014, 590, Kuang, Z.; Chen, Y.; Lu, Y.; Liu, L.; Hu, S.; Wen, S.; Mao, Y.; Zhang, L., Fabrication of Highly Oriented Hexagonal Boron Nitride Nanosheet/Elastomer Nanocomposites with High Thermal Conductivity. Small 2015, 11, Yuan, C.; Duan, B.; Li, L.; Xie, B.; Huang, M.; Luo, X., Thermal Conductivity of Polymer-Based Composites with Magnetic Aligned Hexagonal Boron Nitride Platelets. ACS Appl. Mater. Interfaces 2015, 7, Zeng, X.; Yao, Y.; Gong, Z.; Wang, F.; Sun, R.; Xu, J.; Wong, C.-P., Ice-Templated Assembly Strategy to Construct 3d Boron Nitride Nanosheet Networks in Polymer Composites for Thermal Conductivity Improvement. Small 2015, 11, Kim, K.; Ju, H.; Kim, J., Vertical Particle Alignment of Boron Nitride and Silicon Carbide Binary Filler System for Thermal Conductivity Enhancement. Compos. Sci. Technol. 2016, 123, Kim, K.; Kim, J., Vertical Filler Alignment of Boron Nitride/Epoxy Composite for Thermal Conductivity Enhancement Via External Magnetic Field. Int. J. Therm. Sci. 2016, 100, Yao, Y.; Zeng, X.; Wang, F.; Sun, R.; Xu, J.-b.; Wong, C.-P., Significant Enhancement of Thermal Conductivity in Bioinspired Freestanding Boron Nitride Papers Filled with Graphene Oxide. Chem. Mater. 2016, 28, S-13