Halloysite nanotubes (HNTs) have attracted a technologic and scientific attention as reinforcements of epoxy-based nanocomposites. However, their reported interaction with epoxy matrices is varied and the controlled dispersion of HNTs is still a challenge. In this work, we study the effect of chemical reactions taking place in the dispersion process of halloysite and their possible influence in the composite's properties. HNTs' surface was modified through an alkaline treatment and by grafting two aminosilanes with different chain lengths and functionality numbers. Evidence of homopolymerization and degradation reactions was found, depending on the surface treatment. The rheological study indicated that an interconnected network can be achieved in epoxy/HNTs blends depending on the surface chemical characteristics of the nanofillers and the blending method. The better dispersion was accomplished when ultrasonicating with the aid of a solvent. Nevertheless, the mechanical properties of the nanocomposites are not warranted by selecting a dispersion method.During the last decade, scientists and engineers have discovered and developed a large range of exciting new applications for these unique, cheap, and abundantly available naturally occurring clays. 17,18 Regarding the production of reinforced polymers, one key factor needed to obtain a composite material that successfully fulfill the required service life performance, is to control nanofiller dispersion and nanofiller/matrix interaction. Due to their lower number of surface hydroxyl groups, it is expected that HNTs will disperse better than other silicates such as montmorillonite and kaolinite. It is reported that HNTs can be dispersed quite uniformly by a direct melt-blending Additional Supporting Information may be found in the online version of this article.