Catalysis is the essential technology for precisely transforming the chemical structure of matter on a large scale. It lies at the heart of our quality of life, and it is also essential to a healthy economy. One of the main challenges for catalysis in the 21st century is to better understand and thereof design new catalyst structures in order to control more efficiently the catalytic activity, selectivity and stability. It is thus necessary for France to move forward and to develop innovative catalysts in order to “stimulate industrial revival”. Designing catalytic nano-architectures offers the promise of higher activity, selectivity and stability, provided the following specifications are followed: i) a precise control of nanoparticle (NP) size or shape, ii) a control of the direct environment of the NP, and iii) a robust and controlled (covalent) metal-support interaction. This is far from being the case on conventional supported catalysts, since particle size distributions are often quite broad, and due to the complex support surface chemistry, the nature of the metal support interaction is not precisely controlled, resulting in non-optimized catalytic performances. The ICARE_1 project focuses on the design of totally innovative heterogeneous catalysts. Inspired by Metal-Organic Frameworks, we propose to develop a totally original family of hybrid materials, named metal-carbon frameworks (MECAFs), associating in a controlled manner and through covalent bonds, sp2–C and sp3–C nanostructured carbon materials with metallic NPs. The nanostructured carbon materials selected include C60 fullerenes and molecular nanodiamonds (NDs) derived from adamantane and diamantane. The controlled functionalization of nanocarbons in combination with the covalent bonding should ensure directionality in the assembly; chains (1D), planar (2D) or 3D assemblies are targeted. Additionally, the kinetic/thermodynamic control of the reaction should allow the construction of metallic NPs atom per atom, which is up until now impossible. This material should thus combines: i) a controlled NP size (an atom per atom NP construction is aimed), ii) an atomically-defined environment for the NPs, iii) a covalent interaction with the support, and iv) a high porosity and a highly dense surface area availability of the catalytic centers. To reach this objective, an interdisciplinary approach is necessary; we thus strongly rely on consortium expertise for: i) the synthesis and functionalization of C60 and NDs, ii) the synthesis and characterization of metallic NPs for which metals such as Au, Ru and Pd are targeted because of their valuable catalytic applications, iii) the controlled assembly of hybrid structures, and iv) a computational approach aimed at modelling and understanding the formation of such mixed edifices construction. We will apply MECAFs to a strategic domain of catalysis in industrialized countries: fine chemical synthesis. Two reactions of high industrial interest have been selected, for which catalytic activity, selectivity and stability are genuine challenges: i) the hydroaminomethylation reaction that allows producing amines from alkenes, and ii) the direct arylation of unactivated C–H bonds in heteroaromatics that sustainably bring diversity in fine chemicals synthesis. We will specifically search information linking structure and reactivity/selectivity. Such a groundbreaking material assembly would be very innovative, and the potential for scientific and technological progresses is enormous. Besides catalysis, MECAFS should be of great interest for chemists and physicists. For example, the study of the magnetic and transport properties of magnetic MECAF should be very exciting for physicists. For chemists, the chemical reactivity of atomically defined NPs is an exciting perspective. Additionally, the possibility to reach high metal loading and high dispersion offer interesting perspectives for electrocatalysis or for gas storage.