Dust depositions are critical archives for understanding interior aridification and westerly climatic changes in Central Asia. Accurate and reliable dating of loess is very important for interpreting and correlating environmental records. There remains a disparity between luminescence ages and radiocarbon dating of late Quaternary loess from the Ili Basin in Central Asia. In this study, we establish a closely spaced quartz optically stimulated luminescence (OSL) chronology for the 20.5-m-thick Nilka loess section in the Ili Basin. Based on OSL ages, two intervals of higher mass accumulation rate occurred at 49–43 ka and 24–14 ka. We further compare these OSL ages with 23 accelerator mass spectrometry (AMS) 14C ages of bulk organic matter. The results indicate that the OSL and radiocarbon ages agree well for ages younger than ca. 25 14C cal ka BP. However, beyond 30 cal ka BP, there is no consistent increase in AMS 14C age with depth, while the OSL ages continue to increase. These differences confirm the observation that the AMS 14C ages obtained using conventional acid–base–acid (ABA) pretreatment are severely underestimated in other terrestrial deposits in Central Asia, which could be due to 2–4% modern carbon contamination. However, OSL dating is applicable for constructing an accurate chronology beyond 30 cal ka BP. We suggest caution when interpreting paleoenvironmental changes based on radiocarbon ages older than 25 cal ka BP.