Hierarchical architectures consisting of small building blocks of inorganic crystals are widely found in biominerals. Crystal growth mimicking biomineralization has been studied using various kinds of organic molecules and molecular assembly. The emergence of complex organization of inorganic crystals was observed through biomimetic approaches in aqueous solution. A wide variety of hierarchical architectures including fractals, dendrites, self-similar and helical structures were achieved in the artificial systems. Self-organized formation, with exquisite control of mass transport and the variation of surface energy with organic molecules, is essential for versatile morphogenesis of inorganic crystals similar to biominerals.