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A facile method for the shape-selective synthesis of silica nanostructures using a reverse-microemulsion-mediated template (RMMT) technique is reported. In this method, positive poly- l -lysine (PLL) is selected as template due to its configuration diversity. By adjusting pH and concentration, PLL demonstrates various secondary structures containing random coil, α -helix and β -sheet, which result in the formation of silica nanorods, silica nanospheres and silica nanotubes in the reverse-microemulsion system, respectively. Thus, the shape-selective synthesis of silica nanostructures might be achieved by using PLL as structural template in the reverse-microemulsion system.