AbstractInorganic‐organic hybrid materials with redox‐active components were prepared by an aqueous precipitation reaction of ammonium heptamolybdate (AHM) with para‐phenylenediamine (PPD). A scalable and low‐energy continuous wet chemical synthesis process, known as the microjet process, was used to prepare particles with large surface area in the submicrometer range with high purity and reproducibility on a large scale. Two different crystalline hybrid products were formed depending on the ratio of molybdate to organic ligand and pH. A ratio of para‐phenylenediamine to ammonium heptamolybdate from 1 : 1 to 5 : 1 resulted in the compound [C₆H₁₀N₂]₂[Mo₈O₂₆] ⋅ 6 H₂O, while higher PPD ratios from 9 : 1 to 30 : 1 yielded a composition of [C₆H₉N₂]₄[NH₄]₂[Mo₇O₂₄] ⋅ 3 H₂O. The electrochemical behavior of the two products was tested in a battery cell environment. Only the second of the two hybrid materials showed an exceptionally high capacity of 1084 mAh g⁻¹ at 100 mA g⁻¹ after 150 cycles. The maximum capacity was reached after an induction phase, which can be explained by a combination of a conversion reaction with lithium to Li₂MoO₄ and an additional in situ polymerization of PPD. The final hybrid material is a promising material for lithium‐ion battery (LIB) applications.