In this work, we introduce anisotropically shaped, ultrathin micro- and nano-capsules fabricated by layer-by-layer approach. The original cubic and tetrahedral shapes of the template particles were replicated to produce hollow capsules with well-defined edges. Introducing tannic acid as a component of LbL shells resulted in enhanced chemical stability of these hollow polymer structures under a wide pH range due to high pKa value. Computational studies demonstrated increased mechanical stability of the anisotropic capsules under osmotic pressure variation due to sharp edges and vertices acting as a reinforcing frame in contrast to spherical microcapsules that undergo random buckling. The anisotropic shape of inorganic crystals was precisely reproduced to create hollow cubic and tetrahedral polymeric capsules based on hydrogen-bonded LbL multilayers. The capsules demonstrated excellent integrity and capability to preserve the shape in solution after core removal as well as high pH and mechanical stability as revealed by experimental and simulation studies. Copyright © 2010 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.