Polyoxometalates (POMs), anionic nanosized oxoclusters that can be considered as fragments of metal oxides, have been extensively studied for their diverse composition and structure, showing promise in various fields such as catalysis and electronics. Proton conduction, relevant to catalysis and electronics, has attracted interest in materials chemistry, and POM anions are advantageous in terms of their proton carrier density and mobility. Recently, polar POMs have attracted attention for their unique ferroelectric behaviors, yet they have been little studied with regard to proton conduction, as their polarity has generally been believed to have a negative impact. Here, we propose that polar POMs can be used to align polar proton carriers, such as H