Ultrathin sheets of transition metal dichalcogenides have received a great deal of interest in an attempt to develop advanced electrode nanomaterials for electrochemical capacitors, with most of the attention focused on pure transition metal dichalcogenides. We systematically investigated and compared the charge storage capability of tert-butyllithium-exfoliated group 6 transition metal dichalcogenide materials (MX2; M = Mo, W; X = S, Se, Te). The group 6 MX2 2D materials exhibited distinctive charge storage performance as a result of their different chemical compositions and morphological features. MoTe2 nanosheets demonstrated the highest gravimetric capacitance of all materials. Furthermore, we hybridized these 2D materials with nanofibrous polyaniline (PANI) to study the impact of MX2 materials on its capacitance performance. All the fabricated nanocomposites exhibited a greatly enhanced capacitance compared with the pure PANI, with the highest increase observed for MoTe2/PANI (499 F g−1), which represents a 76% increase. This enhancement arises from the promotion of available active surface area of PANI and MoTe2 for electrolyte ions.