Achieving a sustainable chemical future will require the development of efficient processes for the interconversion of electrical and chemical energy for renewable fuels production, fuel cell applications, and the synthesis of chemical feedstocks. Molecular transition metal electrocatalysts often operate with high selectivity under mild operating conditions, and offer precise control over the active site through systematic tuning of the ligand and metal complex properties. In the first part of my talk, I will discuss our efforts to use hydride transfer to promote the electrochemical oxidation of fuels and the electrochemical reduction of organic substrates. We have developed a family of cobalt-phosphine complexes that facilitate electrocatalytic formate oxidation at mild potentials and high selectivity. By tuning the complex coordination sphere and the reaction conditions, we reveal trends in the thermodynamic properties, catalyst stability, and rate of formate oxidation. I will also present our recent work to develop electrochemical ionic hydrogenation for the reduction of carbonyl compounds using an iridium catalyst. The selective reduction of acetophenone can be achieved using Brønsted acids at mild applied potentials, and Lewis acids induce a significant rate increase. In the final part of my talk, I will share our work using redox-active ligands to promote multielectron redox behavior at first-row metal complexes. We have shown that a class of cobalt-phenylenediamide complexes undergo reversible two-electron oxidation, which can be tuned over 0.5 V. Experimental and computational studies were used to establish the electronic structure of these complexes. The application of these systems to promote small molecule activation via ligand-to-substrate electron transfer or ligand-based hydrogen atom transfer will be discussed.