Rational hybridization of two-dimensional (2D) nanomaterials with extrinsic species has shown great promise for a wide range of applications. To date, rational design and engineering of heterostructures based on 2D metal-organic frameworks (MOFs) has been rather limited. Herein, we report an efficient strategy to construct noble metal/2D MOF heterostructures, featuring the utilization of surface oxygen sites from uncoordinated MOF ligands. The incorporation of highly dispersed noble metal nanoparticles (e.g., Pt and Pd) with modulated electronic structure is enabled on a surfactant-free MOF surface. As a proof-of-concept demonstration, the 2D Ni-MOF@Pt hybrid with well-defined interfaces is applied to boost the electrochemical hydrogen evolution reaction (HER) and delivers decent electrocatalytic activity under both acidic and alkaline conditions. The present results are expected to provide new insights into furnishing MOFs with extended functionalities and applications.