The temperature dependency and reversibility of the sheet resistance of silver nanoparticles covered by 3-mercaptopropionic acid (Ag-MPA) molecules, used in the printed temperature sensor, has been investigated. The microstructural evaluation, the FTIR spectra and thermal property analyses of the Ag-MPA films suggest co-existence of both weakly adsorbed as well as firmly adsorbed MPA molecules on the surface of Ag nanoparticles. The weakly adsorbed MPA molecules was to a great extent be desorbed and removed from the surfaces of silver nanoparticles when heated up to 180 °C for the first time. While the firmly adsorbed MPA molecules remain on the surfaces of silver nanoparticles even at higher temperature. Yet the firmly adsorbed MPA molecules are likely having gone through a transformation circle from/to the gauche and trans conformations in correspondence to a heating and cooling cycle, which results in temperature dependent and reversible sheet resistance. The MPA molecules in the gauche conformation are more densely packed on the surface of silver nanoparticles and can hinder the electron’s movability within the Ag-MPA film. While in the trans conformation with lower ‘surface space’ coverage by the MPA molecules, electrons move more freely within the film. Based on the temperature dependent nature, the fully printed temperature sensor using the Ag-MPA nanoparticles as the functional layer was made, of which the highest sensitivity is 5.12% °C−1 at 200 °C.