High hydrogen capacity (up to 2.6 wt%) is reported for highly aligned structures of Graphene oxide-Multiwalled carbon nanotubes composite at room temperature. It is demonstrated that the scalable liquid crystal route can be employed as a new method to prepare unique 3-D framework of graphene oxide layers with proper interlayer spacing as building blocks for cost-effective high-capacity hydrogen storage media. The strong synergistic effect of the intercalation of MWCNTs as 1-D spacers within graphene oxide frameworks resulted in unrivalled high hydrogen capacity at ambient temperature. The mechanisms involved in the intercalation procedure are fully discussed. The main concept behind intercalating one-dimensional spacers in between giant GO sheets represents a versatile and highly scalable route to fabricate devices with superior hydrogen uptake.