Loess–palaeosol sequences serve as valuable archives of changes in climate and atmospheric mineral dust deposition. However, little work has been conducted on Holocene loess in the Arctic, despite the sensitivity of this region to climate changes. Aeolian silt/loess profiles in the ice-free region of western Greenland near Kangerlussuaq were sampled to develop a robust age framework using both luminescence and bulk organic matter radiocarbon dating. Radiocarbon ages generally show consistent age increases with depth but are likely offset to younger ages due to sediment mixing in the upper 10–20 cm of the profiles. Quartz OSL signals exhibit insensitivity, while low-temperature infrared stimulated luminescence performed at 50 °C (IR50) and the post-IR IRSL at 180 °C (pIRIR180) signals of polymineral fine grain revealed a consistent natural inherited dose of approximately 5 Gy for pIRIR180 and an unbleachable residual of around 2 Gy for IR50, with substantial fading rates in the latter. This led to a notable age overestimation when compared with bulk organic matter radiocarbon ages. To develop an appropriate dating approach, we evaluated the differential bleaching rates of feldspar IR50 and pIRIR180 signals, and corrected for modern inherited doses. Radiocarbon ages measured on the bulk organic carbon oxidised at 400 °C (LT 14C) increased very consistently with depth, allowing calculation of accumulation rates. The presence of the atmospheric radiocarbon bomb signal at depth indicated down-mixing of surface material into the profile, which caused negative (younger) age offsets. The offset-corrected radiocarbon-based age-depth model could be compared to the luminescence results. We show that a combination of LT 14C with polymineral pIRIR180 dating allows the development of age models for these deposits. This multi-chronological approach reveals that loess accumulation in the region was initiated around 4 ka, probably consisting of two main phases of loess accumulation at 4–3 ka and <1 ka. The initial phase matches the proposed onset of aeolian sand activity in the wider region, but post-dates local ice retreat by c. 3 kyr. The more recent phase of accumulation also matches the timing of increased sand accumulation in the region and likely coincides with Neoglacial to Little Ice Age ice advances, or even enhanced dust activity in the last decades.