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Advanced hybrid nanomaterials (nanohybrids) with unique tailored morphologies and compositions have been used for the targetoriented catalysts due to the structural or supportive properties of each moiety and the synergistic properties of the individual components.The rational design and development of nanohybrids by integrating highly porous silica into a nano metal-organic framework (NMOF) are expected to enable unique nanospace engineering in the resulting systems to optimize their utility in the target areas.Herein,we report the design and fabrication of advanced nanohybrids composed of dendritic fibrous nanosilica (DFNS) and DFNS/gold (DFNS/Au) hybrids as the core and zinc-based NMOF (Zn-NMOF) as the shell (DFNS@Zn-NMOF)through a solution-based approach.The combined fibrous morphology of DFNS and micropores of NMOF can be directly employed for nanospace engineering in the resulting multi-compositional and hierarchical systems in a controllable manner.The DFNS/Au dots@Zn-NMOF nanohybrid shows improved catalytic performance in the Knoevenagel condensation reaction,attributed mainly to the cooperative effect stemming from the suitably organized configurations of each component.