This proposal is focused on the synthesis of novel non-conventional inorganic and porous catalytic materials, in the latter explicitly focusing on supramolecular-organic frameworks (HOFs), their enzymatic biocomposites, and fourth-generation metal-organic frameworks (MOFs), multivariate and composite MOFs not present in the literature. We will exploit innovative and green synthetic strategies to prepare these materials, such as advanced mechanochemical and vapor-solid reactions. In this context, a key objective is to design and build advanced mechanochemical reactors that combine plasma and mechanical forces to synthesize the coordinative and supramolecular catalysts. These reactors will also transform inorganic catalysts and milling media, which will be evaluated for catalytic applications. All materials will undergo thorough characterization using laboratory and synchrotron techniques and computational methods. The catalytic performance of selected materials will be assessed for key environmental processes, such as biomass remediation and carbon dioxide reduction, and heterogeneous catalysis to produce added-value chemicals. We will establish the kinetic details of the promising processes by in situ monitoring methods using synchrotron diffraction and Raman spectroscopy. To enhance the understanding of these processes, a novel in situ monitoring technique will be developed to track the luminescent material syntheses, which are challenging to capture with conventional Raman spectroscopic approaches. The best-performing materials will be scaled to pilot scales using batch (drum mill) or continuous mechanochemical processing by extrusion. The project involves a strong international network of collaborators with expertise in advanced analytical and catalytic methods. Young researchers will gain hands-on experience and expand their skills through collaborative exchanges, strengthening their competitiveness in the global research landscape.