Many MOFs can be synthesised with a range of different particle morphologies and three-dimensional pore networks, as well as different degrees of particle agglomeration. While significant work has examined the impact of pore structure on the capacitive performances of porous carbon materials and other families of electrically conductive MOFs, little work has been performed to understand how morphology impact the performances of layered MOFs in supercapacitors. This has hindered the development of layered MOF for energy storage applications, with potential performance gains to be had from optimising the microstructure. One notable exception is the work of Dincă et al., which studied the influence of microstructure on the capacitive performance of Ni3(HITP)2 (HITP = 2,3,6,7,10,11-hexaiminotriphenylene) in three-electrode cells with 1 M KOH in water electrolyte. This study suggested that samples with smaller length-to-width aspect ratio particles ('flatter' crystals) and lower levels of particle agglomeration display superior capacitive performances compared to samples with both larger length-to-width aspect ratio particles and greater agglomeration. However, this work primarily relied on batch-to-batch variation to synthesise different samples. This resulted in relatively small differences in observed microstructure, with a variation in the length-to-width aspect ratio over the range of 2.7 -12.1, and small changes in agglomeration. Inspired by this study, we were interested in systematically synthesising layered MOFs with a broader range of controlled microstructures, and then using these to comprehensively study the impact of electrode microstructure on electrochemical performance.