Nanostructures loaded on halloysite nanotubes (HNTs) have attracted global interest, because the nanotubular HNTs could extend the range of their potential applications. In this study, we fabricated a novel nanocomposite with hollow iron nanoparticles loaded on the surface of HNTs. The structure of the iron nanoparticles can be adjusted by ageing time. Owing to the increased remnant magnetization and coercivity values, the nanocomposites loaded with hollow iron nanoparticles showed better electromagnetic performance than that with solid iron nanoparticles. This study opens a new pathway to fabricate halloysite nanotubular nanocomposites that may gain applications in the catalytic degradation of organic pollutants and electromagnetic wave absorption.