LAUSR

Conductive polymers (CPs) are arranged in the end‐on direction on graphene surfaces using 3D tectons of ZnPc assemblies, to control carrier transport from hot to cold via external magnetic fields. Poly(3,4‐ethylenedioxythiophene)s doped with tosylate are synthesized using monomer seeds that are complexed through pyridine units to 3D tectons on graphene via surface‐confined host‐guest chemistry, to provide an end‐on‐oriented polymer film on graphene with a high degree of crystallinity. The film shows free‐electron‐like charge transport properties, with an enhanced Hall mobility, and an increased Seebeck coefficient compared to the CP on graphene that is prepared without 3D tectons. A magneto‐thermoelectric (MTE) effect is reproducibly observed for the film device. Taking advantage of a large photothermal effect of the polymer film, a photon‐mode MTE effect is demonstrated for the first time. Both dark and photo‐MTE effects correlate well to the generated Lorentz force. These results provide a unique tool to program carrier transport in thin‐film via external magnetic stimuli with a temperature gradient.