In the context of green chemistry, cascade catalytic reactions appear as ideal solutions for industry. Combining strategies from biocatalysis to chemocatalysis, the Ni(k)AGARA project aims at experimentally demonstrating the concept of cascade catalysis in cristallo on oxidative transformations of alkenes, performed in multi active sites cross-linked artificial enzyme crystals (CLEC). It will consist of an evolution of our mastered CLEC application that will require innovative chemical modifications in NikA protein crystals for the insertion of a second inorganic catalytic site. Our knowledge in high performance of alkenes’ degradation using dioxygen as oxidant will drive us to add downstream transformations in an original cascade of catalytic oxidation reactions, implying carbonation, aldehyde oxidation, or degradation of polyunsaturated biomolecules. Never performed on hybrid solid catalysts, such a catalytic process could eventually reach the requirements for an industrial use. he project is divided into two main objectives: first, the construction of two catalytic sites within a protein, distinguished by their mode of insertion. The first will be based on supramolecular interactions as mastered by the consortium today, while the latter will be covalently linked to the solvent channels of the protein crystal. the method of attachment will be obtained by the mutation of an amino acid of the N-terminal chain with a cysteine; this one will then react with related functions on the ligand of the metal complex to integrate. An alternative will be to perform click chemistry on an unnatural azido amino acid. Catalysis of transformation will be the second objective, a choice resulting from the recent discoveries of the consortium. Oxidative cleavage of alkene has been shown to be catalytic with artificial protein crystals, based on the insertion of iron complexes within the NikA protein. On this basis, the activation of CO2 will be undertaken in the second stage of the cascade reaction: a transformation of epoxides into carbonates or the subsequent oxidation of polyenes are an illustration of this. The interdisciplinary project Ni(k)AGARA deals with the conception of innovative solutions for a sustainable chemistry. It will cover research at the interface of biotechnology and chemistry. Accordingly, the project concerns basic science to develop new catalytic solutions for green chemistry, involving a bio-inspired design of heterogeneous biocatalysts. The outstanding quality of the present project relies into the right combination between sustainability and catalysis, creating new innovative solutions for catalysis while targeting pollutants, or bio-based molecules building blocks. The scientific benefits will be numerous at various levels. Firstly, the consortium will develop new tools to transform chemically crystalline proteins and understand the catalytic mechanisms at molecular level. Secondly, the application for polymer transformation should open new greener routes. Accordingly, it fulfills the requirements of “stimuler le renouveau industriel” and should be evaluated by the CES “chimie moléculaire, chimie durable et procédés associés” since catalysis is associated to eco-efficiency and to the development of new molecules. A second reading level of the project deals with the search of new reactions processes for high value products combining the valorization of CO2 with polymer functionalization, a very active field for polymers with low environmental impacts. Partner 1 and 2 have been involved in collaborative projects since 2008 and their common publications in journals of high impact attest of their efficacy. Partner 3 will afford its knowledge in CO2 activation and polymer science, making the targeted reactions eventually appreciable by the industry world and open a new field of possibilities for this original catalytic approach.