The increasing number of commercial, technological and scientific missions for CubeSats poses several concerns about the topic of space junk and debris mitigation. As no regulation is currently in place, innovative solutions are needed to mitigate the impact that Low Earth Orbit objects can have during uncontrolled re-entry and the associated potential events of surface collision. We investigated the requirements, in terms of materials selection, for the development of a 3D-printed structural bus able to withstand loads during launch and in-orbit operations, with the objectives to be as light as possible and requiring the least amount of heat for demise during atmospheric re-entry. The selection indicated magnesium alloys as the best candidates to improve the reference material, aluminium 6061 T6, resulting in both mass-reduction and improved demisability. We also analysed how the relative importance of these two objectives can modify the selection of materials: if minimizing the heat to disintegration were valued more highly than lightness, for example, the new best candidates would become tin alloys. Our analysis, furthermore, suggested the importance of Liquid Crystal Polymer as the sole plastic material approaching the performance of the best metal choices. This contribution, thus, provides novel insight in the field of 3D-printed materials for the fast-growing CubeSat segment, complying with the debris mitigation initiatives promoted by space agencies and institutions.