The combination of pillarization and charge neutralization with Li + can make montmorillonite an important support material for industry and decontamination of pollutants in soil and water. Montmorillonite characterization techniques were described in detail, and pillarization procedures were used, after Li + saturation, to modify and manipulate the chemical and mineralogical surface properties of this montmorillonite. Eight samples were produced: 1) natural montmorillonite (Chisholm Mine - MMT); 2) Li+ saturated montmorillonite (MMTLi); 3) polyethylene glycol (PEG) Al-pillared montmorillonite (AlPEG); 4) PEG Al-pillared montmorillonite saturated with Li (AlPEGLi); 5) Al-pillared montmorillonite with 14 h contact time (Al14h); 6) Al-pillared montmorillonite Al14h saturated with Li (Al14hLi); 7) Al-pillared montmorillonite with 0 h contact time (Al0h); and 8) Al-pillared montmorillonite Al0h saturated with Li (Al0hLi). The natural sample was identified as interlayered montmorillonite composed of chlorite layers or with a high degree of Al-hydroxy filling. Concerning the total permanent charges, 70 % occurred by isomorphic substitution of Al 3+ by Mg 2+ in octahedral layer and 30 % of Si 4+ by Al 3+ in tetrahedral layer. The pillarization method using the PEG produced a small number of stable pillars. The new milder pillarization method (Al0h) did not cause damage in the formation of Al-hydroxy. In this method, the resulting pillars were more homogeneous in size. Thereby, the Al0h Li method has been shown to produce a supporting material with a constant interlayer spacing, increased of the specific surface area (SSA), and drastic reduction of the cation exchange capacity (CEC) as compared to MMT. This modified mineral can be used in, for example, decontamination of polluted water with nonionic organic pollutants.