Nickel particles with a highly ordered mesostructure are prepared by electroless deposition of Ni salts dissolved in aqueous domains of lyotropic liquid crystalline (LLC) media made of a nonionic surfactant (Brij 56) at a high concentration. The mesostructure inside the Ni particles after the electroless deposition has a macroscopic alignment of mesochannels derived from the LLC media which are composed of crystalline domains on a micrometer scale. It is proved that the arrangements of rod-like self-assemblies in the LLC indeed work as a scaffold to direct the grain growth of Ni. This is the first direct evidence of direct physical casting from LLC. (c) 2005 The Electrochemical Society.