Supplementary Information Extremely anisotropic single crystal growth in nano-twinned copper Chia-Ling Lu 1, Han-Wen Lin 1, Chien-Min Liu 1, Yi-Sa Huang 1, Tien-Lin Lu 1, Tao-Chi Liu 1, Hsiang-Yao Hsiao 1, Chih Chen 1, Jui-Chao Kuo 2 and King-Ning Tu 3 1 Department of Materials Science & Engineering, National Chiao Tung University, Hsinchu, 30010, Taiwan, R.O.C. 2 Department of Materials Science & Engineering, National Cheng Kung University, Tainan, 70101, Taiwan, R.O.C. 3 Department of Materials Science and Engineering, University of California at Los Angeles, Los Angeles, CA, 90095, U.S.A Correspondence: Professor Chih Chen, Department of Materials Science & Engineering, National Chiao Tung University, Hsinchu, 30010, Taiwan, R.O.C. E-mail : chih@mail.nctu.edu.tw (C. Chen). Figure S1 (a) Plan-view focused ion beam (FIB) image showing the as-fabricated <111> film. (b) Plan-view FIB image of a large <100> grain that grew among the <111> grains after annealing at 450 °C for 10 min. (c) Enlarged FIB image for the dashed rectangle in b. 1 Figure S2 (a) Plan-view FIB image for the as-fabricated <111> Cu crystals with a diameter of 100 m. (b) Plan-view FIB image for nine <100> Cu crystals after annealing at 450 °C for 60 min. Figure S3 (a) and (b) Cross-sectional FIB images for the sample with all of the <111> grains transformed into large <100> crystals. 2 Figure S4 Cross-sectional FIB images for the sample after annealing at 400 °C for 20 min. Figure S5. The statistics results showing the number fraction of grains as a function misalignment angle from the [100] direction. (a) for the grains in Fig. 10a; (b) For the grains in Fig. 10c. (c) For the grains in Fig. 5d;The average misorientation angle was 3.0, 2.8, and 4.7 degree for the [100]-oriented grains in Fig. S5a, S5b, and S5c, respectively. 3