This study is focused on the catalytic activity of monometallic and bimetallic Al-MCM-41 supported Ce and Zr heterogeneous catalysts prepared by impregnation and co-impregnation methods, respectively. Physicochemical properties of the catalysts determined, such as N2 adsorption isotherms and X-ray diffraction (XRD) studies show that the catalysts were mesoporous aluminosilicates with disordered hexagonal structure. The prepared catalysts were applied in simultaneous esterification and transesterification reactions of Jatropha oil for biodiesel production. The bimetallic catalyst was found to be more active than both the monometallic catalysts and the support. The bifunctional activity of the synthesized catalysts was observed at varied reaction conditions. Influence of the reaction conditions shows the highest conversion of biodiesel was obtained at methanol to oil ratio 6:1, reaction temperature 90 °C, reaction time 4 h and catalyst loading 5 wt%. The high performance of the bimetallic catalyst in the reaction process is attributed to optimum regulation of active sites by both Ce and Zr metals on the surface of the catalyst. Results from the GC-FID chromatograph shows the successful conversion of triglyceride to methyl esters.