The orientation of polymer chains and supramolecular nanostructures plays significant roles in determining the final properties of polymer materials. Typically, the orientation of polymer chains can be controlled by applying external fields (e.g., mechanical force, electric field, magnetic field, and light) or epitaxy to polymer materials during processing. In this contribution, we demonstrate that the orientation of polymer chains and supramolecular nanostructure can be well controlled by confinement. Two-dimensional confinement is achieved by embossing crystallizable polymer thin films into hard templates bearing nanoscale channels and subsequent crystallization. It is found that the fast growth direction of polymer nanocrystals, i.e., the long axis of the nanocrystals, is aligned parallel to the nanochannels defined in the hard templates under full confinement due to graphoepitaxial or entropic effects. In addition, the high internal order in the polymer nanostructures can translate into lower coercive field and higher piezoelectric coefficient d33 in ferroelectric poly(vinylidene fluoride-co-trifluoroethylene) (PVDF-TrFE)1-4, and into higher charge transport mobility in conjugated polymers5-7. References: 1. Y. Wu, X. Li, Y. Weng, Z. Hu, A. M. Jonas, Polymer 2014, 55, 970. 2. H. G. Kassa, L. Nougaret, R. Cai, A. Marrani, B. Nysten, Z. Hu, A. M. Jonas, Macromolecules 2014, 47, 4711. 3. L. Nougaret, H. G. Kassa, R. Cai, T. Patois, B. Nysten, A. J. J. M. van Breemen, G. H. Gelinck, D. M. de leeuw, A. Marrani, Z. Hu, A. M. Jonas, ACS Nano 2014, 8, 3498. 4. Y. Wu, X. Li, A. M. Jonas, Z. Hu, Phys. Rev. Lett. 2015, 115, 267601. 5. G. Ding, Y. Wu, Y. Weng, W. Zhang, Z. Hu, Macromolecules 2013, 46, 8638. 6. G. Ding, C. Li, X. Li, Y. WU, J. Liu, Y. Li, Z. Hu, Y. Li, Nanoscale 2015, 7, 11024. 7. S. Wei, Y. Zhang, J. Liu, X. Li, Y. Wu, H. Wei, Y. Weng, X. Gao, Y. Li, S.-D. Wang, Z. Hu, Adv. Mater. Interfaces 2015, 1500153.