Focusing on molecular perovskites, our results have important ramifications on how to think and approach the challenge of designing molecular perovskites with targeted mechanical properties and, more generally, targeted network distortions. Evidently, A + templates framework distortions, and when aiming for large distortions, A + should be chosen that largely diverges from a sphere. For A + based on alkylated ammonium or phosphonium, a chemical functionalisation that enables the formation of conformers with large anisotropies seems fruitful. This suggests the use of a more rigorous conformational analysis prior to the synthesis of A + cations. In parallel, robust criteria for describing the asphericity of A + should be tested, where we consider G as an important yet only qualitative measure since any templating effect can be expected to be related to asphericity and volume. Such developments have the potential to bring related fields to fruition, such as the targeted design of active distortion modes, with implications for the synthesis of improper ferroelectrics.