Some efforts have been made to synthesize high-quality halloysite-like nanotubes during the last decades (Gardolinski and Lagaly, 2005 and Kuroda et al., 2011). As high-quality kaolinite is readily available at low cost, one of the most attractive methods for synthesizing aluminosilicate nanotubes is based on the delamination and rolling of kaolinite layers. This process might have drawn inspiration from the observation of the kaolinite–halloysite transformation occurring in nature. For example, Giese (1988) reported that kaolinite formed from mica by topotactic alteration could subsequently produce halloysite. Singh and Gilkes (1992) described the electron-optical observation of the alteration of kaolinite plates by fragmentation into laths that rolled to form halloysite tubes. Bobos et al. (2001) confirmed the kaolinite to halloysite transformation by comparing the clay samples selected from the same geological profile in a Portuguese kaolin deposit. The theoretical studies on the rolling mechanisms of halloysite have further accelerated improving the methods for halloysite preparation.