AbstractSelf‐assembly of asymmetric amphiphiles containing an azobenzene unit selectively produces molecular monolayer nanotubes, which can act as solid supports for enzymes without the use of chemical cross‐linkers. Encapsulation of enzymes in nanotube channels and continuous capping of both open ends with magnetic nanoparticles allow us to construct bioreactors. Transformation of the nanotubes to nanocoils induced by the trans‐to‐cis isomerization of the azobenzene unit upon UV‐light irradiation initiates catalysis due to the appearance of multiple narrow slits functioning as size‐exclusion pathways for penetration of substrates from bulk solution. Kinetic performance of encapsulated enzymes is similar to that of free enzymes. Magnetic nanoparticles are very useful for inhibiting the release of encapsulated enzymes and conferring magnetic properties to organic nanotubes and nanocoils. Simple recovery and separation with a magnet allow high reusability and recyclability of the bioreactors; in addition, nanotubes and nanocoils stabilize the encapsulated enzymes. The bioreactors work well even in the presence of proteases, which are able to eliminate the catalytic activity of enzymes in bulk solution.