Organocatalysis is a rapidly expanding methodology enabling challenging chemical transformations to be performed in the broad context of sustainable chemistry (metal-free procedures, catalyst recycling…) in line with Challenge 3, CS07 of the ANR Work Program 2018. Despite major achievements, organocatalysts generally suffer from low rate acceleration and turnover and the need for relatively high amounts to achieve good conversion and selectivity. This project which involves three academic laboratories in France and one in Spain, with a strong and unique complementarity, is aimed at developing original catalytic systems utilizing the chiral micro-environment of oligourea helices to catalyze challenging asymmetric transformations at (very) low catalyst loading. Particular attention will be paid to mechanistic studies to elucidate the mode of action of these helical oligomers with the aim to optimize their performance and further expand their reaction and substrate scope.