This work transfers the basic concept of functionalization reaction in organic chemistry to inorganic chemistry, which promotes the fusion of organic and inorganic synthetic chemistry. It opens the door for the bottom-up synthesis of organic-inorganic hybrid materials from hybrid molecules, pushing forward the control of hybrid material structures at molecular precision. The molecular scale covalent-ionic bicontinuous network suggests a new hybrid structure to combine paradoxical properties within one material, which broke the performance compromise in conventional composites. As Nature senior editor Kristina Kareh said, “The paper is a true demonstration of a new class of material”. Maybe in the near future, the hybrid molecules generated by the functionalization of inorganic ionic oligomers are expected to be used for the bottom-up design of more hybrid materials and these materials with new properties may open new application fields.