Clay is a natural material constructed from the tetrahedral silica sheet and octahedral alumina. The most important minerals in clays are those that have layered structures and are classified as phyllosilicate. Phyllosilicate is structured lattice silicates which are formed from a series of silica tetrahedral sheets with octahedral alumina bonded due to oxygen atoms used together. Among the most commonly used phyllosilicate clay minerals for making pillared layered solids is the montmorillonite group (bentonite). Montmorillonite attracts a lot of attention as it has the ability to expand (swell) has exchangeable cations and can be intercalated. Montmorillonite is included in the smectite group, having molecular formula Nax[Al(x-2)Mgx(Si4O10)(OH)]· mH2O [1,2].It is easy to expand nature and its ability to exchange ions through the cations exchange mechanism are potential key points for clay modifications. The modifications inferred include intercalation, which is the replacement of ions between the silicate layers with the cationic polymer in the form of organic Bentonite as a carrier was modified by means of pillarization using ZrOCl2·8H2O pillaring solution. Calcination was performed to obtain ZrO2 bounded bentonite. To create a bifunctional catalyst, ZrO2-bentonite was impregnated using Ni(NO3)2·6H2O precursor as nickel metal source. Subsequently, calcination and reduction steps were performed to obtain Ni/ZrO2-bentonite catalyst. The physical-chemical properties of catalyst was characterized by XRD, XRF and the surface area was analyzed with BET, surface acidity with gravimetric method using NH3 vapour, FT-IR and TEM. The characterized results by XRD showed specific peaks of montmorillonite mineral still visible after the pillarization and impregnation process with nickel metal. The XRD analysis also showed an increase in basal spacing d001 of the catalyst sample after the pillarization process characterized by the shifting of specific peaks d001 to the left (2θ < 5º). The XRF analysis showed that the nickel content in bentonite sample was increased after impregnation with the Ni(NO3)2·6H2O precursor. Qualitatively, acidity of the catalysts was determined by FTIR showing characteristics for Brønsted and Lewis acids at wavenumbers 1635-1381 cm -1 . Surface area analysis results showed an increase in specific surface area after pillarization and impregnation with nickel metal.This is an open access journal, and articles are distributed under the terms of the Creative Commons Attribution-NonCommercial 4.0 International (CC BY-NC 4.0) License, which allows others to copy and redistribute the material in any medium or format, remix, transform, and build upon the material, as long as appropriate credit is given and the new creations are licensed under the identical terms.