Fast-growing worldwide energy demand and a significant impact on air pollution with increasing emissions of greenhouse gas carbon dioxide (CO2) are resulting in global warming and human health issues. New technologies need to be developed urgently that can directly convert CO2 with excess electricity from sustainable sources (solar, wind) into storable fuels and chemicals. The major obstacles to convert CO2 into energy-bearing products is the high stability of the CO2 mole-cule and the lack of efficient catalysts. Electrocatalysis is an attractive, low temperature catalytic pro-cess for the reduction of CO2 because it activates CO2 by direct input of electrical energy. Only a few products, such as CO and formic acid, have been produced selectively and with some acceptable pro-duction rates through the electrocatalytic CO2 conversion (ECR), using state of the art catalysts. The next step towards the (direct) fabrication of “CO2 neutral fuels” in a sustainable energy system is the development of more efficient and selective CO2 reduction catalysts. This PhD thesis aims to develop and implement bimetallic catalyst structures into carbon nano-fiber architectures for electrocatalytic CO2 reduction, including research on MOF derived nanofiber catalysts as gas diffusion electrodes (GDEs). The project is an Alliance project with Technion, a leading partner university of DTU in Israel.