Gaining external control over self-organization is of vital importance for future smart materials.S urfactants are extremely valuable for the synthesis of diverse nanomaterials. Their self-assembly is dictated by microphase separation, the hydrophobic effect, and head-group repulsion. It is desirable to supplement surfactants with an added mode of long-range and directional interaction. Magnetic forces are ideal, as they are not shielded in water.W er eport on surfactants with heads containing tightly bound transition-metal centers.T he magnetic moment of the head was varied systematically while keeping shape and charge constant. Changes in the magnetic moment of the head led to notable differences in surface tension, aggregate size, and contact angle,which could also be altered by an external magnetic field. The most astonishing result was that the use of magnetic surfactants as structuredirecting agents enabled the formation of porous solids with 12-fold rotational symmetry.The spontaneous formation of organized patterns as an intrinsic property of asystem containing discrete constituents, ap rocess termed self-assembly,h as fascinated scientists for decades.N ature shows the enormous potential of such behavior, since many of the unexcelled properties of biological matter originate from its capacity for adaptive selfassembly.[1] Full exploration of this potential in materials science is still remote,a smost reported examples of selfassembly so far are dictated by internal factors,s uch as thermodynamic equilibrium.[2] Systems reaching as tate of higher order only under constant consumption of energy (dissipative,n on-equilibrium state) have seldom been reported.[3] Apremise for advancing research in this direction is that compounds capable of adaptive self-assembly can be equipped with the ability to be actuated externally.Examples from particle research, such as dispersions of superparamagnetic colloids, [4] demonstrate the promise of manipulation by the use of magnetism, because it can be applied in astatic or dynamic way,a nd unlike electric fields,m agnetism is not damped in aqueous electrolytes.T hus,i ti sw orth exploring the use of external magnetic fields to trigger the selforganization of molecular systems.As model systems for the self-assembly of soft matter, surfactants are the focus of much current interest. Surfactants are molecular species that contain two moieties of opposite solvent compatibility arranged in adipolar geometry.Inpolar solvents,u sually water, concentration-dependents elf-organization takes place.T he amphiphilic properties of surfactants make them suitable for the stabilization of interfaces of many kinds,f or example,f or the generation of nanoparticles or nanoporous materials.[5] Thetypical head group of surfactants is organic in nature and, thus,d iamagnetic.T om ake as urfactant magnetic, one of its constituents should contain ap aramagnetic metal species.T his emerging field was reviewed very recently by Eastoe and co-workers.[6] Most known examples involve surfac...