Nowadays, the analysis of volatile organic compounds (VOCs) is very important in various domains. For this, in the last decades, electronic noses have emerged as promising alternatives to traditional analytical methods. Nevertheless, their wide use is still limited by their performances such as low selectivity. Herein, we developed an optoelectronic nose using virtually screened peptides and hairpin DNA (hpDNA) with improved selectivity as sensing materials and surface plasmon resonance imaging (SPRi) as the detection system. Thanks to the complementarity of their binding properties towards target VOCs, the obtained optoelectronic nose has very good selectivity, being able to discriminate not only between VOCs of different chemical families, but also VOCs of the same family with only 1-carbon difference. We thus confirmed that computational virtual screening, which allows 'in silico' testing of VOC-peptide binding in a fast and low-cost way, is very promising for the selection of sensing elements with higher sensitivity and selectivity as well as great diversity. The combination of these sensing materials with SPRi is relevant for the development of optoelectronic nose with large sensor arrays and improved performances.