Metal-organic frameworks (MOFs) are potentially useful molecular materials that can exhibit structure flexibilities induced by some external stimuli. Such structure transformations can furnish MOFs with improved properties. The shape-controlled growth of MOFs combined with crystal-structure transformation is rarely achieved. Herein, we demonstrate the synthesis of hierarchical Zn/Ni-MOF-2 nanosheet-assembled hollow nanocubes (NAHNs) by a facile surfactant-free solvothermal approach. The unique nanostructures undergo crystal-structure transformation from Zn/Ni-MOF-5 nanocubes to Zn/Ni-MOF-2 nanosheets, which is analogous to the dissolution and recrystallization of inorganic nanocrystals. The present synthetic strategy to fabricate isostructural MOFs with hierarchical, hollow, and bimetallic nanostructures is expected to expand the diversity and range of potential applications of MOFs.