To investigate the influence of microstructure on the energy storage performance of Cu3(HHTP)2, three samples of Cu3(HHTP)2 were synthesised with ammonia, dimethylformamide (DMF) and pyridine as modulating agents, respectively (Fig. ). It has been well studied that varying the identity of the modulator is an effective way to regulate particle morphology and agglomeration, with the different modulators thought to lead to distinct framework growth mechanisms and kinetics due to differing interactions with the Cu(II) ions and organic linker molecules in the reaction mixture. Ammonia, DMF and pyridine were chosen as the modulating agents for this study as previous work indicated that these modulators would produce samples with distinctly different microstructures, including in both particle morphology and the degree of agglomeration. This allows for a more robust investigation into the influence of microstructure on the capacitive performance of layered MOFs than previously possible.