Gas-phase bioproduction, in which immobilized biocatalysts are employed and chemical reactions are performed in a gas phase, has attracted researchers’ attention as a green process. However, there is difficulty in the employment of whole cell catalysts for gas-phase bioproduction due to the lack of a suitable cell immobilization method. <i>Acinetobacter</i> sp. Tol 5 is a unique bacterium, which is remarkably sticky and can be easily immobilized onto various material surfaces through the adhesive bacterionanofiber protein AtaA. In this study, we demonstrate the gas-phase bioproduction of (<i>E</i>)-geranic acid (GA), a high-value-added monoterpenoid, from geraniol using immobilized Tol 5 transformant cells, into which a gene involved in a (<i>E</i>)-GA synthetic pathway was introduced. Time course analysis of the liquid-phase bioproduction of (<i>E</i>)-GA revealed the inherent metabolism of Tol 5 involved in the degradation of (<i>E</i>)-GA. By disrupting the <i>fadD4</i>-ortholog gene, which encodes a key enzyme of the (<i>E</i>)-GA degradation, we successfully generated a (<i>E</i>)-GA-accumulating strain, Tol 5 Δ<i>fadD4</i> (pGeoA). The immobilized cells of this mutant strain on a polyurethane support enabled the production of (<i>E</i>)-GA with a passive supply of gaseous geraniol in a batch gas-phase reaction. A major fraction of the (<i>E</i>)-GA, which was produced, was adsorbed onto the polyurethane support but easily extracted into ethanol, a safe solvent without environmental impact. This is the first example of gas-phase bioproduction of a complex and high-value-added compound. Tol 5 is a highly promising platform for gas-phase bioproduction.