As is widely known, the construction industry is one of the sectors with a large contribution to global carbon emissions. Despite numerous efforts in the construction industry to develop low-carbon materials, there is a limited number of studies quantifying and presenting the overall environmental impact when these materials are applied in a construction project as structural members. To address this gap, this study focuses on assessing the life-cycle performance of novel structural aluminium alloy–concrete composite columns. In this paper, the environmental impacts and economic aspects of a concrete-filled aluminium alloy tubular (CFAT) column and a concrete-filled double-skin aluminium alloy tubular (CFDSAT) column were assessed using life-cycle assessment (LCA) and life-cycle cost analysis (LCCA) approaches, respectively. The cradle-to-grave system boundary is considered for these analyses to cover the entire life-cycle. A concrete-filled steel tubular (CFST) column is also assessed for reference. All columns are designed to have the same load-carrying capacity and, thus, are compared on a level-playing basis. A comparison is also made of the self-weight of these columns. In particular, the self-weight of the CFST column is reduced by around 17% when the steel tube is replaced by an aluminium alloy tube, and decreased by 47% when the double-skin technique is adopted in CFDSAT columns. The LCA results indicate that the CO2 emission of CFST and CFAT is almost the same, which is 21% less than the CFDSAT columns due to the use of high aluminium in the latter. The LCCA results show that the total life-cycle cost of CFAT and CFDSAT columns is around 29% and 14% lower, respectively, than that of the CFST column. Finally, a sensitivity analysis was carried out to evaluate the effects of data and assumptions on the life-cycle performance of the examined columns.