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Reliable models of the lung environment are important for research on inhalation products, drug delivery, and how aerosols interact with tissue. pH fluctuations frequently accompany real physiological processes in pulmonary environments, so monitoring pH changes in lung-on-a-chip devices is of considerable relevance. Presented here are flexible, miniaturized, inkjet-printed pH sensors that have been developed with the aim of integration into lung-on-a-chip systems. Different types of functional pH-sensitive materials were tested: hydrogen-selective plasticized PVC membranes and polyaniline (both electrodeposited and dropcast). Their deposition and performance were evaluated on different flexible conducting substrates, including screen-printed carbon electrodes (SPE) and inkjet-printed graphene electrodes (IJP-Gr). Finally, a biocompatible dropcast polyaniline-modified IJP was selected and paired with an inkjet-printed Ag/AgCl quasireference electrode. The printed potentiometric device showed Nernstian sensitivity (58.8 mV/pH) with good reproducibility, reversibility, and potential stability. The optimized system was integrated with a developed lung-on-a-chip model with an electrospun polycaprolactone membrane and alginate, simulating the alveolar barrier and the natural mucosal environment, respectively. The permeability of the system was studied by monitoring the pH changes upon the introduction of a 10 wt.% acetic acid aerosol. Overall, the presented approach shows that electrospun-hydrogel materials together with integrated microsensors can help create improved models for studying aerosol transport, diffusion, and chemically changing environments that are relevant for inhalation therapy and respiratory research. These results show that our system can combine mechanical behavior with chemical sensing in one platform, which may be useful for future development of lung-on-a-chip technologies.