Chiral templating and enantioselective separations are demonstrated on graphene surfaces as directed by encapsulated silica nanotubes. Electrostatic assembly of helical silica nanotubes within graphene sheets results in a hybrid material with the electrochemical properties of graphene and the capability for chiral recognition. Control of the silica nanotube helicity within the graphene hybrid provides a means for directed chiral templating of guest molecules on the outer graphene surface as revealed in the chiral transcription of <i>N</i><sup>1</sup>,<i>N</i><sup>3</sup>,<i>N</i><sup>5</sup>-tri(4-pyridinyl)cyclohexane-1,3,5-tricarboxamide as well as polyallylamine into supramolecular templated assemblies. Changing the helicity of the internal nanotube also provides control over enantiomer selectivity as demonstrated by the chiral separation of racemic mixtures of phenylalanine, tryptophan, and alanine derivatives