In addition, we have modelled the fracture behaviour using an X-ray CT based chemomechanical finite element model that shows a clear link between primary particle anisotropy and significant cracking at elevated voltages. We predict crack initiation in the centre of the particle at approximately 4 V that propagates outwards as voltage increases -this is commensurate with the experimental evidence. Excessive cracking at 4.5 V can be directly linked with the collapse of the c-lattice, at which point the primary particles undergo aggressive contraction that generates tensile stresses at the joints between their neighbours. This technique could be applied to other chemistries including single crystal and solid state electrolytes as a an easy way to confirm the origin of cracking and the cracking tendencies in these materials. In addition, phase contrast imaging could be used in the future to resolve the carbon binder domain of the electrode and elucidate any contribution to secondary particle cracking that may be missed here. For all next generation chemistries looking to be employed in EVs, it is paramount to understand the cracking and loss of conductive contact behaviour to help mitigate these and prolong the lifetimes of cells, which may contribute to a reduction in battery wastage as they become more prominent in the automotive industry.