The domain configurations and local piezoresponse property of the [720]‐cut BaTiO3 single crystal and [001]‐oriented BaTiO3 crystal were investigated by high‐resolution piezoresponse force microscopy. Large differences in their surface topography features, domain configurations and local piezoresponse were found between [720]‐cut and [001]‐oriented BaTiO3 crystals. The large surface bending angle due to ferroelastic domain walls leads to a high strain energy appearing in the [720]‐cut BaTiO3, further resulting in unique band‐like topographic features, needle domains for stress compensation and locally ultrahigh piezoelectric response as well. (© 2013 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)