Display omitted •Zeolites included in the nanofibers increased the adsorption capacity of model VOC.•Silicalite type of zeolite adsorbed 60 % higher amount of model VOC.•Up-scaling of the process with a 150 fold increase of formed CA/UHSZ nanofibers.•Diffusion of ammonia vapours is not influenced by the structure of the material. The optimized preparation of novel electrospun nanofibrous composites from cellulose acetate (CA) and ultra-high silica zeolites (UHSZ) are reported as a promising material for the adsorption of Volatile Organic Compound (VOCs). Two types of UHSZs, i.e. silicalite and USY were prepared by hydrothermal crystallization while the fabrication of composites was performed using single needle and needle-less electrospinning systems, demonstrating the scalability of the composite fibres’ manufactured. Herein, factors such as properties of spinning solutions and electrospinning process parameters were studied, as well as interactions between the CA and UHSZs. In addition, Quartz Crystal Microbalance - Dissipation technique (QCM-D) was employed with an aim to study the adsorption behaviour of newly developed composites using ammonia as a model pollutant. The QCM-D data revealed that the presence of UHSZs in the CA materials increased adsorption capacity, designating CA/UHSZ composites as potential materials suitable for a large-scale removal of VOCs from polluted air.