This study introduces a versatile one-pot hydrothermal synthesis strategy that enables simultaneous control of MoS2 structure over several length scales, ranging from macroscopic crystallite size to microscopic lattice parameter control. Lowering the pH of the precursor solution for hydrothermal synthesis leads to the formation of smaller crystallites. The addition of alkyldiamines like 1,6-hexanediamine (HDA) of different lengths to the same precursor solution will lead to their confinement between the forming MoS2 layers, acting as structural pillars expanding MoS2 interlayer spacing. By changing the HDA concentration, the content of structural pillars in interlayer-expanded MoS2 can be varied to some extent. The interaction between HDA pillars and MoS2 host is purely physical in absence of covalent bonding, with no significant crystallographic changes in the MoS2 in-plane structure after pillaring.