Advances in computational modelling now offer an efficient route to developing novel helmet liners that could exceed contemporary materials' performance. Furthermore, the rise of accessible additive manufacturing presents a viable route to achieving otherwise unobtainable material structures. This study leverages an established finite element-based approach to the optimisation of cellular structures for the loading conditions of a typical helmet impact. A novel elastomeric pre-buckled honeycomb structure is adopted and optimised, the performance of which is baselined relative to vinyl nitrile foam under direct and oblique loading conditions. Results demonstrate that a simplified optimisation strategy is scalable to represent the behaviour of a full helmet. Under oblique impact conditions, the optimised pre-buckled honeycomb liner exceeds the contemporary material performance when considering computed kinematic metrics head and rotational injury criterion, by up to 49.9% and 56.6%. Furthermore, when considering tissue-based severity metrics via finite element simulations of a human brain model, maximum principal strain and cumulative strain density measures are reduced by 14.9% and 66.7% when comparing the new material, to baseline.