Nowadays, there is a growing demand for the analysis of volatile organic compounds (VOCs) in various domains, including environment, quality control, and medical diagnostics. Traditional analytical methods, though accurate and reliable, require expensive equipment and are often time-consuming and laborious. On the other side, food & fragrance industries employ human sensory panels to evaluate the quality of an odour. However, panellists are expensive to train and employ and they can give biased results. To bridge the gap, we developed different sensor systems inspired by the human nose. Here, a biomimetic olfactory biosensor based on key-and-lock principle was designed using odorant binding proteins as receptors for the analysis of few VOCs in liquid. In parallel, an optoelectronic nose based on cross-reactive principle was developed for sensing various VOCs in the gas phase. For both systems, surface plasmon resonance imaging (SPRi) was employed since it allows monitoring interactions in a label-free and real-time manner with a temporal response, which is particularly interesting for the electronic nose development. For the olfactory biosensor, a conventional and commercial SPRi set up was used. In contrast, for the optoelectronic nose, we developed a homemade SPRi dedicated for gas sensing by combing with a cross-reactive array, for the first time. The obtained olfactory biosensors showed a good selectivity to β-ionone with a detection limit among the lowest reported in the literature, regarding both the VOC concentration (3.6 x 10-10M) and the VOC mass (100 Da) detected by SPRi. Our optoelectronic nose was very effective in sensing VOCs of different families with an extremely high selectivity, capable of discriminating between homologous VOC analytes with a single carbon resolution. Therefore, these systems are promising alternatives for the analysis of VOCs with potential applications in various domains.