The well-developed design strategy of molecular modification for assembling molecular ferroelectrics mainly focuses on the cations. Herein, by homochiral anionic modification of the non-ferroelectric (quinuclidinium)(HSO₄), we designed high-temperature multiaxial organic enantiomeric ferroelectrics, (quinuclidinium)(L- and D-camphorsulfonate). This work paves a new road for precisely constructing excellent molecular ferroelectrics.