Tuning the physical and chemical interaction between metal-metal' (M-M') and metal-support is an ideal way to realize enhanced catalytic activity of metal nanoparticles (NPs). As a proof of concept, herein we report the fabrication of nickel-gold (Ni-Au) alloy nanoparticles attached to N-doped nanoporous carbon (NPC) intervened with MgO (Ni73Au27@MgO-NPC), achieved through the impregnation of metal precursors into Schiff-base network polymer (SNP) framework along with Mg(OH)2 and pyrolysis at 800 °C in N2 atmosphere. With high stability and heterogeneity, the nickel rich Ni73Au27@MgO-NPC exhibited higher catalytic activities with turnover frequencies of 29,272 h-1 (hydrogenation of p-nitrophenol), 93,843 h-1 (degradation of methyl orange), and 2,218 h-1 (epoxidation of stilbene), compared to commercial 10 wt % Pd/C. Enhanced catalytic activity is correlated to the synchronized electron density enhancement in Au, by Ni and MgO/N-rich nanoporous carbon heterostructures, as evident from detailed X-ray photoelectron spectroscopic studies.