In this work, we propose a potentiometric smart sensor for lithium detection in environmental samples based on a screen-printed cell. The graphite screen-printed electrode (GSPE) was first modified by gold and silver nanoparticles to increase the conductivity, and then by an ion-selective membrane, which was directly deposited onto the nanostructured electrode surface. The potentiometric cell, thanks to its small size, was integrated with a portable instrument connected to a smartphone for decentralized analysis. The developed sensor was used in drop- and microflow-configurations and showed a high sensitivity for lithium with a low detection limit (1.6 µM). It was also applied in the analysis of real samples from the industrial recycling of automotive batteries and complex matrices, such as contaminated soils.