The structural characterization of HDA-pillared MoS2 materials demonstrated that the materials exhibit an expanded interlayer spacing compared to nano-MoS2, while other structural properties like morphology, crystallite size and in-plane MoS2 structure remained similar. Furthermore, the concentration of HDA pillars is increased in MoS2-HDA-1 compared to MoS2-HDA-0.5. Consequently, the materials can be used to study the influence of (1) interlayer spacing (i.e., nanoconfinement geometry) and ( a low initial Coulombic efficiency (ICE, 44 %) is observed, which is correlated to the above described 2H-to-1T phase transformation in the plateau region around 1.1 V vs. Li + /Li during the first lithiation (Fig. ). In comparison, both MoS2-HDA-1 and MoS2-HDA-0.5 exhibit higher ICEs of 65 % and 67 %, respectively, in absence of the 2H-to-1T phase transformation plateau. Instead, they likely undergo a 1T'-to-1T transformation during the first lithiation (vide infra). The initial anodic (delithiation) capacities of nano-MoS2 and MoS2-HDA-1 are in the same range (182 and 178 mAh/g, respectively), while the delithiation capacity of MoS2-HDA-0.5 is increased to 199 mAh/g. Given that these values are normalized to the full composite mass of MoS2 and HDA, the capacities of HDA-pillared materials significantly exceed that of nano-MoS2 per transition metal (221 mAh/gMoS2 or Li1.38-MoS2-HDA-1; and 237 mAh/gMoS2 or Li1.48-MoS2-HDA-0.5). This is in line with previous reports of increased Li + storage in interlayer-expanded MoS2 materials that potentially combines pseudocapacitive (Faradaic) Li + intercalation with an additional electric double-layer capacitance inside the widened interlayer galleries and/or at the solid/liquid interface. Cyclic voltammograms of interlayer-expanded MoS2 electrodes show an increased capacitorlike, rectangular current profile and the absence of the broad redox peak around 1.7 -1.9 V vs. Li + /Li as compared to nano-MoS2 (Fig. ). Given the lower content of electrochemically inactive HDA-pillars in MoS2-HDA-0.5, its specific current signal has a slightly higher magnitude