Due to the large proliferation of electrical devices combined with the ecological transition for carbon neutrality in various modern countries, the demand for compact and efficient portable energy sources is continuously increasing. In this research work, we have developed electrochemical energy storage heterostructures based on graphene oxides (GOs) and titanium disulfide (TiS2) nanosheets of different lateral sizes through a facile colloidal association thanks to the opposite electric charges of the two types of nanosheets. Large GO (LGO) served as a template system to organize TiS2 nanosheets at different loadings, of which incorporation prevented any restacking of the layered graphitic structure. While large nanosheets led to the decoration of TiS2 aggregates including Li+ cations on LGO, the association of the nanosheets of different compositions but equivalent sizes drove the formation of an interstratified organization of the nanosheets. The singular organization within GO and TiS2 nanosheets remained after a hydrothermal reduction process, leading to heterostructure materials with a large specific surface area and capacitance of 113 F/g obtained in 6 M KOH aqueous solution. These outstanding electrochemical performances, drastically enhanced by about 41% from those of the individual reduced GO (capacitance of 80 F/g) used as a collector for the electric carriers, suggest that the developed heterostructures present a possible application as electrochemical energy storage technology materials for supercapacitor applications.