It is important to monitor and detect volatile organic compounds (VOCs) for environmental protection, occupational safety and human health. Portable and compact VOC sensing devices with a fast response are needed for real-time monitoring and simple analysis. Using solvent exchange and freeze-drying techniques, an ultralight 3D bacterial cellulose (BC) aerogel is prepared and modified by polyethylene glycol with the functionalization of graphene and metal oxides to detect VOC gases. Unlike commercially available flat VOC sensors, the 3D structure of our VOC sensor with high permeability of BC composite provides superior sensing characteristics for acetone, formaldehyde and ethanol in a wider range of scenarios. The portable BC composite sensor exhibits remarkable sensitivity and selectivity toward VOCs detection. The BC composite with TiO2 has a response time of about 20 s to 1 ppm acetone and can detect as low as 1.43 ppm at room temperature. In addition, BC composites with ZnO are suitable for detecting formaldehyde in indoor air.