AbstractPrecise adjustment of microstructure and handedness of chiral nanomaterials is important to regulate their properties and performance. Herein, helical 3‐aminophenol formaldehyde resin (APF) nanotubes and corresponding carbonaceous nanotubes with controllable handedness and optical activity were obtained via an external metal ion‐mediated supramolecular co‐templating method in an enantiomerically pure template system, in which an appropriate amount of Mn2+ (Co2+ or Ni2+) with moderate coordination abilities can reverse the spatial arrangement of the phenylglycine‐based amphiphilic template molecules through metal coordination. Different stacking modes of coordination complexes in disparate metal ion systems lead to diverse helical senses (diameter and pitch) of the obtained helical APF. In addition, this coordination mode of metal intervention can be applied to other amine‐based helical polymer synthesis systems, which paves the way for the design of high‐quality chiral nanomaterials with satisfactory physical parameters and properties.