Combination of antiāresonant hollowācore fiber (HCF) and semiconductor nanomaterial is an effective strategy to obtain highāperformance gas sensors with exceptional sensitivity and low power consumption. However, controlling the semiconductor morphology onto HCF is a major challenge to achieve the desired gas sensor with the enhanced sensitivity. Here, a ZnOāBi2O3 nanosheets (NSs) heterostructure is grown in situ on the surface of HCF by solāgel and hydrothermal methods. ZnOāBi2O3 NSs serving as electron acceptors trap electrons after acetone adsorption and then change the refractive index of the surface of HCF. Benefiting from the unique sheet structure and the synergetic effects for multiācomponent, the resulting ZnOāBi2O3 NSs enabled HCF gas sensor exhibits high sensitivity, selectivity, and repeatability for detecting acetone at room temperature, particularly in the low concentration range, with the theoretical limit of detection down to 140 partsāperābillion. Meanwhile, the successful application of the ZnOāBi2O3 NSs enabled HCF gas sensor to distinguish the exhaled breath from the healthy individuals and simulated diabetic cases is demonstrated, which paves the way to achieve nonāinvasive, ultraāsensitivity gas sensing at room temperature for the early diagnosis of diabetes.