Metallosalen complexes are able to catalyze several transformations via a bimetallic, cooperative pathway. Various strategies to induce simultaneous activation by two metal centers with multinuclear catalysts have been reported to date, leading to higher reaction rates and selectivities in existing reactions. In some cases, new reactions could be realized that were previously not possible. The design principles, the most successful approaches and the catalytic applications of multinuclear metallosalen catalysts are discussed in this feature article.