A modulated synthesis of Zr-metal organic framework (Zr-MOF) with improved ease of handling and decreased reaction time is reported to yield highly crystalline Zr-MOF with well-defined octahedral shaped crystals for practical hydrogen storage applications. The Zr-MOF obtained from the modulated synthesis showed high thermal and moisture stabilities with enhanced hydrogen storage capacity. Further study suggests that the modulated synthesis of Zr-MOF may lead to the development of a flow-through synthesis process. Copyright (C) 2013, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.