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A localized surface plasmon resonance gas sensor based on Au nano-island films coated with molecularly imprinted polymer (MIP) layer was developed to selectively detect terpene vapor emitted from plants. Au nano-islands were deposited on a glass substrate through repeated Au sputtering and annealing. The MIP layer was coated on Au nano-island films by spin-coating a pre-polymerized solution containing methacrylic acid as monomer, ethylene glycol dimethylacrylate as cross-linker, and \alpha -pinene as the template molecule. The influence of nanostructure on the refractive index (RI) sensing characteristics was mainly investigated in this paper. The result demonstrated that the structure of Au nano-island films could be controlled by Au sputtering-annealing cycle. Increase in the sputtering-annealing cycle induced the size increase and the inter-particle distance decrease of Au nano-island films. In addition, spectral red shift, decrease in transmittance, and increase in absorbance were observed under this procedure as well. The typical RI sensing evaluation parameters \Delta \lambda _{\mathrm {{max}}} , \Delta \text{T}_{\mathrm {{min}}} , and \Delta \textA\mathrm {{max}} achieved the maximum values: 9.75 nm, and 9%, 0.42 under 3 and 18 Au sputtering-annealing cycles. Au nano-island films under 3 and 18 Au sputtering-annealing cycles were coated with the MIP, and the response of MIP-coated Au nano-island sensor to \alpha -pinene vapor was verified to be fast, reversible, and reproducible. [ABSTRACT FROM PUBLISHER]