Natural sources display a high potential for the production of sustainable materials because of their exceptional structural and physical features, nontoxicity, biocompatibility, availability and cost-effectiveness. Nanostructured systems show high surface/volume ratio, and unusual electrical, mechanical, surface and magnetic properties. The preparation of heterogeneous nanocatalysts from natural resources has recently become increasingly attractive for researchers. The present overview discuses extensively and comprehensively the main natural sources used to prepare the new generation of safer and cheaper catalytic nanosystems. We place a significant emphasis on both the different synthetic strategies for the preparation of the Nature-inspired nanocatalyst and the role of the natural materials over the structural and morphological properties of the resulting nanocatalysts. The catalytic applications of nature-inspired materials were finally featured, highlighting the advantages of using nanotechnology and environmental resources as well as their potential towards the production of alternative energies.