The aim of this study was to characterise the microstructural organisation of staple carbon fibre-reinforced polymer composites and to investigate their mechanical properties. Conventionally, fibre-reinforced materials are manufactured using continuous fibres. However, discontinuous fibres are crucial for developing sustainable structural second-life applications. Specifically, aligning staple fibres into yarn or tape-like structures enables similar usage to continuous fibre-based products. Understanding the effects of fibre orientation, fibre length, and compaction on mechanical performance can facilitate the fibres’ use as standard engineering materials. This study employed methods ranging from microscale to macroscale, such as image analysis, X-ray computed tomography, and mechanical testing, to quantify the microstructural organisations resulting from different alignment processing methods. These results were compared with the results of mechanical tests to validate and comprehend the relationship between fibre alignment and strength. The results show a significant influence of alignment on fibre orientation distribution, fibre volume fraction, tortuosity, and mechanical properties. Furthermore, different characteristics of the staple fibre tapes were identified and attributed to kinematic effects during movement of the sliver alignment unit, resulting in varying tape thicknesses and fuzzy surfaces.@en