In this work, a new ionic liquid (IL) with two acidic and vinylic functional groups based on 1,2,3benzotriazolium cation was synthesized. This IL monomer was intercalated into the montmorillonite (MMT) layers by the ion exchange reaction and subsequently copolymerized with the IL monomer and methacrylic acid in order to obtain positive charge pH-sensitive nanocomposites. The structure of the IL monomer was characterized by FT-IR and 1 H-NMR spectroscopy, and the structure of the nanocomposites was studied and confirmed by the FT-IR, XRD, TGA, SEM, and EDX data. These pH-sensitive nanocarriers were used to load and in vitro release of the anticancer drug, methotrexate (MTX) in pH = 4 and pH = 7.4. The results showed that the release is pH dependent and more effective in acidic pH; therefore, these nanocarriers have potential to be used for cancer therapy.