Polyaniline composites with graphene and graphene oxide have received broad interest for applications in charge separation and storage in electrical devices. Syntheses via in situ polymerization of aniline in colloidal dispersions of graphene oxide have afforded nanocomposites of polyaniline intercalated within graphene oxide nanosheets. The simultaneous inclusion of LAPONITE® nanoparticles has improved aqueous phase processability and thin film formation. Mechanical, morphological and conductivity studies including atomic force microscopy and scanning electron microscopy were employed to study the host–guest interactions and heterointerfaces that govern self-assembly. Adhesion and conductivity values within graphene oxide/polyaniline/LAPONITE® (GOPL) nanocomposites were tuned by varying the weight ratios of polyaniline : graphene oxide. These studies inform ongoing work to use GOPL nanomaterials for clean energy harvesting and storage applications.