D-π conjugated coordination polymers (CCPs) are often widely used in photocatalysis and electrocatalysis due to their unique electronic conductivity and structural flexibility. However, it remains a challenge to overcome the self-degradation of d-π CCPs in thermal catalysis and to effectively utilize their excellent electron transfer properties. Here, we present a series of d-π CCPs derivative after calcination treatment. The derivatives were optimized for overall electron cloud density by constructing two-dimensional pyridinic-nitrogen (N) doped carbon carriers, which exhibited the inherent π-electron delocalization and charge transfer properties of d-π CCPs. The presence of electron transfer was confirmed by X-ray Photoelectron Spectroscopy (XPS), Raman and kinetic analysis, demonstrating that this d-π CCPs derivative possesses excellent electron conduction ability and low activation energies for the reaction. Density-functional theory (DFT) calculations further confirmed the modulation of the nickel nanoparticles (Ni NPs) electronic state by the carriers, which resulted in strong Ni NPs interactions with the high-electron-density π-bonds of the CC bond. This property significantly enhances the target adsorption and activation of the CC bond, leading to a substantial enhancement of the reaction performance. This strategy provides a new development direction for the application of d-π CCPs in thermal catalysis.