Carbonyl compounds (CCs) in indoor air pose a significant threat to residents’ health and have garnered considerable attention in recent years. However, most studies have focused on low-molecular-weight carbonyl compounds (LMW-CCs) and have underestimated the impact of high-molecular-weight ones (HMW-CCs), causing a failure to comprehensively understand their effects on health. In this study, we analyzed twenty carbonyls in the indoor and outdoor air at typical residential communities in a megacity in Northwest China by using high-performance liquid chromatography (HPLC) coupled with a photodiode array detector (DAD). The total concentration of indoor carbonyls was 1.4-3.4 times that of outdoor carbonyls. In addition, the concentration of indoor carbonyls was much higher during the heating season than that during the nonheating season. Conversely, the concentration of outdoor carbonyls was higher during the nonheating season than that during the heating season. The principal component analysis (PCA) revealed that indoor carbonyl pollution was primarily influenced by building materials, cooking fume, and wooden furniture. Formaldehyde exposure in indoor environments posed a greater health risk to children than acetaldehyde exposure. HMW-CCs were the primary contributors to indoor odor pollution, which was considered a significant cause of sick building syndrome (SBS). Our findings underscore the crucial role of HMW-CCs in indoor environments in exerting adverse impacts on health.