This talk will provide an overview of our group’s work using both standard and atypical high-performance computational chemistry modeling to elucidate atomic scale reaction mechanisms of catalytic reactions. I will introduce our toolkit of in silico methods for accurately modeling (electro)catalytic reactions in solvating environments. I will then present how in silico methods can be used for predictive insights into chemical and material design. The talk will then highlight our progress in modeling 1) the complex Morita-Baylis-Hillman reaction, 2) inefficient amorphous TiO2 materials as anti-corrosion coatings, and 3) biomimetic CO2 reduction mechanisms.