The synthesis of ionic-mesoporous-metal-organic frameworks (ionic-meso-MOFs) has received considerable interest in the fields of macromolecular adsorption, acid-base catalysis, ionic conductivity, etc.; yet, their synthesis still presents significant difficulties. In this study, functionalized mesoporous MIL-101-ILs (Cr) was facilely constructed via an in situ self-assembly method by using aromatic-anion-functionalized ionic liquids (ILs) as competitive ligands. It has been demonstrated that the inclusion of an aromatic moiety into an IL improves the coordination ability and is advantageous for the anchoring of ILs on Cr3+ via amino-metal coordination. Thus, ionic-meso-MOFs with a specific surface area of 441.9-624.9 cm2/g and an average pore diameter of 5.5 to 8.4 nm were successfully synthesized. Because of the presence of open Lewis acidic metal sites on the MOFs and basic active sites on the ILs, the resulting ionic-meso-MOFs demonstrated both an acid-base cooperative effect and a mesoporous structure, indicating a high potential for acid-base catalysis. This in situ synthesis procedure for ionic mesoporous MOFs offers a simple method for developing and fabricating multifunctional mesoporous materials.