Although the demand for chiral enantiomerically pure molecules as pharmaceuticals, agrochemicals, and liquid crystals is growing strongly, the use of asymmetric catalysis for their production is rare. The most common industrial method to produce enantiopure compounds is still chiral resolution, which wastes half of the material. This surprises considering that catalytic methods are potentially cost-, energy, and resource-saving, have a lesser impact on the environment, and are in line with the general concepts of green chemistry and sustainability. Recently organocatalysis has grown into one of three fundamental classes of asymmetric catalysts complementing metal- and biocatalysis. In principle, organocatalysts have many beneficial features such as air and moisture stability, non-toxicity, and easy accessibility, making them attractive for industrial applications. However, most organocatalysts are insufficiently active and require high catalysts loadings, counterbalancing these positive features. Remarkably, of the four types of organocatalysts, Brønsted bases and acids, and Lewis bases, and acids, organic Lewis acid catalysts have been almost entirely ignored. Very recently though, within the group of the applicant, the finding was made that such catalysts can be extremely active and enantioselective, suggesting the possibility for truly high performance organocatalysis. This proposal therefore aims at the design of novel organic Lewis acid catalysts, their exploration in asymmetric catalysis, and their mechanistic understanding. The program is expected to lead the way towards the next generation organocatalysts, which will rival the efficiency of the most active metal- and biocatalysts, and have the potential to profoundly change the way chiral molecules are made.