Transition to clean energy, mitigation of carbon emissions, and protection of water resources are critical challenges for the world. Solving these challenges requires precise control of many important chemical reactions with sluggish kinetics and myriad possible reaction pathways and associated products. There is a critical need for selective, active, durable and low-cost catalysts. This talk will present our research efforts aimed at bridging the gap between homogenous catalysis and heterogeneous catalysis to realize materials with new or improved electrocatalytic properties for the CO2 and nitrate reduction reactions. Combining molecule-nanocarbon hybridization and second-coordination-sphere tailoring, we discovered the first molecular electrocatalyst for CO2-to-methanol conversion in significant yield and stability. The reduction proceeds via formaldehyde, an intermediate potentially reactive to N nucleophiles. Following this path, we developed the first electrosynthesis of methylamine from CO2 and nitrate. This 15-proton 14-electron reduction reaction proceeds via an 8-step catalytic cascade with the spontaneous condensation reaction between the formaldehyde and hydroxylamine intermediates to form the C-N bond. Further, we advanced the chemistry to ethylamine formation and N-methylation reactions, opening the door for our electrocatalytic reactions to be used for organic synthesis using CO2/nitrate as a C1/N1 building block.