The objective of this study was to explore the geological origin of glauconite, which is believed to precipitate and mature very slowly (~1 Myr) in neritic environments (shallow water, oceanic coastal zones, at water depths of 100–200 m) with very low sedimentation rates. A series of simulation experiments was designed and carried out in sealed tubes placed in an oven and heated to a constant temperature of 50°C (±2°C) for 60 or 150 d. The parent materials used for these experiments were two low-Fe montmorillonites with different crystallinities. The montmorillonites were introduced to solutions with concentrations of 0.02–0.1 mol/L Fe3+and 0.05–0.2 mol/L K+ with various values of pH and Eh. The products were analyzed using X-ray powder diffraction (XRD), Fourier-transform infrared (FTIR) spectrometry, electron spin resonance (ESR) spectrometry, scanning electron microscopy (SEM), and Mössbauer spectroscopy. The morphological changes from parent material to product were observed under SEM, which revealed the formation of a flaky mineral (e.g. a product formed in the interstitial spaces between montmorillonite crystals). The formation of a flaky mineral indicates that the product is a layer silicate. Qualitative analysis of XRD patterns revealed that the main product phase was a mica group mineral and the d060 value was consistent with the presence of glauconite (0.152 nm) and/or Fe-illite (0.150 nm). A glauconite and Fe-illite mineral assemblage formed in a weakly acidic solution, while Fe-illite, mixed-layer Fe-illite, and montmorillonite formed in neutral and alkaline solutions. Stretching vibrations of Fe(III)Fe(III)OH–AlFe(II)OH and/or MgFe(III)OH were observed in FTIR spectra (3550–3562 cm–1) of the products formed in acidic solutions, which along with the g = 1.978 ESR signal indicated that Fe(III) entered octahedral positions in the tetrahedral/octahedral/tetrahedral layer (TOT) platelets. The AlFe(II)OH–MgFe(III)OH (3550–3562 cm–1) and AlFe(III)OH (870 cm–1) vibrations were only observed in products formed in neutral and alkaline solutions. Analysis of the Mössbauer spectra showed that Fe(III) substituted for Al and Mg in the cis octahedral sites of montmorillonite. The simulation experiments demonstrated that the pH and redox conditions (Eh) of the environment controlled the nature of the product mineral species. Results of the present study revealed that glauconitization and illitization occurred under different conditions, where glauconitization preferentially occurred in an acidic environment and illitization preferentially occurred in a nearly neutral to alkaline environment.