This paper reported the preparation of a hierarchical structure consisting of micro-scale basalt fiber fabric and nano-scale carbon nanotubes (CNTs). The developed fabric was employed as reinforcement to develop nanocomposites with multi-layer structures for electromagnetic interference shielding. Different techniques were employed to study the morphologies and properties of the fabric and corresponding nanocomposites. The results showed that by optimizing the experimental conditions, CNTs with controlled content and quality were grown on the surface of basalt fiber. These properties significantly affected the electromagnetic interference shielding performance of corresponding nano composites. The novelty of this study lies in the direct growth of nanotubes on basalt fiber by utilizing the in-situ generated mineral nanoparticles on fiber surface as a catalyst, and a spontaneous infusion of uncured polymer into the fabric, which eliminates the problems associated with the dispersion and re agglomeration of CNTs during the preparation of nanocomposites.