Organic−inorganic hybrid materials (OIHMs) have become a powerful platform for exploring ferroic materials due to the advantages of directional design on the molecular level. Here, based on a hybrid uniaxial ferroelectric (Quinuclidinium)GaCl 4 (QGC), a chiral hybrid (R-3-hydroxylquinuclidinium)GaCl 4 (R3HQGC) was successfully synthesized through a molecular strategy of H/OH substitution. R3HQGC exhibits a much higher Curie temperature (318 K) than QGC (284 K) because hydroxyl modification enhances intermolecular interactions, increasing the movement energy barrier. Meanwhile, R3HQGC shows multiaxiality and multiferroicity (the coexistence of ferroelectricity and ferroelasticity). Notably, R3HQGC has a large spontaneous polarization (19.4 μC•cm −2 ) exceeding those of most multiferroics and multiaxial ferroelectrics. Our study presents an effective approach to promote ferroelectric properties and gives deep insight into exploring high-performance hybrid multiferroic materials.