The synthesis, structural characterization, and electrochemical properties of a series of isotruxenepolyaniline (PANI) hybrid systems (SITPs, SITAs, and CITs) are reported. The syntheses were performed by in situ chemical oxidative polymerization of aniline in the presence of isotruxene additives ITP and/or ITA at specific aniline-to-additive molar ratios. The polymers SITPs and SITAs display granular morphology, but for the polymers CITs a spherical morphology with a diameter of 300-500 nm is found. These hybrid systems display electrochemical capacitive performance superior to those of the parent PANI prepared under the same condition (e.g., 385-463 vs. 181 F/g at 3 mA/cm 2 current density during charge-discharge test). Molecular (star-shaped or hyperbranched vs. linear topology) and supramolecular (isotruxene-PANI π-π and cation-π interactions) models in accounting for the observed morphology and electrochemical properties are provided. . His current researches include (1) Light-and voltage-gated molecular machines; (2) Stimuli-responsive photoluminescent organic and organometallic systems; (3) Electronic properties of π-conjugated oligomers and polymers.