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Polar crystal structures are considered as potential indicators for the design of ferroelectric,piezoelectric,non-linear optical materials,etc.1 The molecule-based materials are an alternated candidate for the design of newpolar crystals because of the flexible designability of their constituent ionic components.2 Herein,twoorganic-inorganic hybrid crystals[quinuclidinium][FeCl4](1) and [quinuclidinium][GeCl3](2) were assembled.