Cryptomelane-type manganese oxide octahedral molecular (OMS) sieve three-dimensional (3D) nanostructures were synthesized via facile temple-free low-temperature hydrothermal reactions. Morphologies of the cryptomelane-type OMS-2 nanoparticles with tunnel dimension of 4.6 × 4.6 Å can be tuned by varying reaction temperatures. At low temperature (120
C), OMS-2 dendritic nanoclusters composed of uniform single-crystal nanotetragonal prisms with square cross-sections were formed. At high temperature (180
C), the morphologies of OMS-2 became spherical dandelion-like microspheres composed of uniform single-crystal OMS-2 nanoneedles. Slow oxidation of Mn
2+ by Cr
2O
7- under hydrothermal conditions is critical for the formation of the hierarchically ordered OMS-2 3D nanostructures.