This study reveals the considerable variety of structural forms that are energetically accessible for lithium halides (LiX, with X = Cl, Br, I) in THF solution. This profusion is due to the intricate pattern governed by the flexibility of the coordination sphere of lithium, the solvent dynamics, and the competition between intramolecular and intermolecular interactions. The wide exploration of the chemical space was made possible only by using an MLP trained on a comprehensive set of AIMD data. In particular, the MLP enabled the investigation of extended timescales with remarkable computational efficiency. These extended time scales were essential in the discovery of possible highly solvated and flexible species. Exploration of the chemical space revealed several key findings. The LiCl species were found to have the largest variety of forms. This free energy surface is essentially flat, containing the emblematic relatively poorly solvated pseudo-cubane and diversely less compact and more solvated species made generally of connected rings of size often larger than four. Additionally, high-weight aggregates of LiCl were studied, where calculations revealed the preference for connected hexagonal units resulting from merging several pseudo-cubanes. The agreement with available experimental structures supports our methodological approach for modeling lithium chloride in solution. Similar calculations for lithium bromide and lithium iodide also showed a great diversity of structures, with a clear tendency to prefer less compact, smaller and more solvated LiX aggregates in which Li• • • X intramolecular interactions are replaced by THF coordination. The structural preferences are proposed to be related to the ionicity of the Li-X bond, which is qualitatively described by the atomic charges. The ionic character decreases from Cl to Br to I, and increases as the size of the LiX aggregates shrinks, with a substantial rise from dimer to monomer. As it is easier for THF to cleave a less ionic Li-X bond, this accounts well for the observed trends. It also accounts for the fact that monomeric LiX is not found to be energetically accessible for any X.