Herein, one-dimensional double helix is fabricated via supramolecular self-assembly of a sugar-based amphiphile, which can be utilized as soft template to synthesize silica double helices and nanotubes through sol−gel reaction of tetraethyl orthosilicate (TEOS). The self-assembled double helix can be rationally transformed into nonhelical fibers with the aid of conventional ionic surfactants. It is suggested that the introduction of ionic surfactant will impart electrostatic repulsion inside double helix and shape double helices into nanofibers. Interestingly the nonhelical fibers coassembled by C4AG and cationic surfactants have been proven to direct the preparation of single-stranded helical SiO2 through sol−gel polycondensation. This is the first time that both double and single-stranded silica helix have been created in one system.