A magnetic surfactant, which combines the properties of a surfactant with magnetic responsiveness, shows great potential in biotechnology, separation, adsorption, and catalysis, especially in noninvasive manipulation through a magnetic field. However, a molecularly magnetic surfactant is usually paramagnetic for the amorphous and less ordered structures. In this work, magnetic surfactant 1-methyl-3hexadecane-imidazolium [MnCl 2 Br] (C 16 M[Mn]) is reported to selfassemble in water. The C 16 M[Mn] magnetic surfactant self-assembles in water to form a lamellar hydrogel from 10 to 50 wt % at and below room temperature. The hydrogel changes from a gel to a sol at 30 °C, and the hexadecane chains in the hydrogel change from noncrystalline to crystalline at 0 °C. In the hydrogel state, the lamellar domain spacing is varied from 36 to 45 nm depending on the concentration and self-assembly temperature. After self-assembly, the magnetic susceptibility of the freeze-dried magnetic surfactant is increased. Most important is the fact that the freeze-dried sample at a high concentration (40−50 wt %) shows the highest magnetic susceptibility, which is related to the closer molecular packing and the more ordered structures. The self-assembly-induced increase in magnetic susceptibility provides a method for improving the magnetic properties of a magnetic surfactant.