A chloride ion selective thin film sensor is proposed for measuring chloride ion concentration, which is an environmental parameter correlated to corrosion. In this work, electrochemical polymerization of Polypyrrole (PPy) doped with chloride ions was achieved on the top of a carbon nanotube (CNT) thin film as a working electrode in an electrochemical cell. The underlying CNT layer conjugated with doped PPy thin film can form a multifunctional “self-sensing” material platform for chloride ion detection in a concrete environment. The paper presents the first type of work using CNT and PPy as hybrid materials for chloride ion sensing. Electrochemical polymerization of PPy results in oxidation that yields an average of one positive charge distributed over four pyrrole units. This positive charge is compensated by negatively-charged chloride ions in the supporting electrolyte. In effect, the chloride ion-doped PPy has become molecularly imprinted with chloride ions thereby providing it with some degree of perm-selectivity for chloride ions. The detection limit of the fabricated chloride ion-doped PPy thin film can reach 10-8 M and selectivity coefficients are comparable to those in the literature. The reported work aims to lay a strong foundation for detecting chloride ion concentrations in the concrete environment.