Effluents from numerous Industries like textile, paint, pharmaceutical, steel and electroplating industries liberate both Zinc [Zn (II)] and Chromium [Cr (VI)] heavy metals. In this work, adsorptive interaction of toxic Zn (II) heavy metal in aqueous solution with synthesized mesoporous silica based MCM‐41 was investigated. Further, the effects of presence of Cr (VI) heavy metal on the adsorption of Zn (II) and vice versa were investigated by simultaneous competitive binary adsorption from Cr (VI) and Zn (II) aqueous binary solution. Batch experiments were executed to see the effects of parameters like pH, adsorbent dose (m), adsorbate concentration and adsorption time (t). Optimum conditions for Zn (II) treatment were obtained as: initial pH (pHi) =7, m=0.1 g/L and t=2 h. Competitive adsorption of both Cr (VI) and Zn (II) from their binary solution was studied at 288− 308 K temperatures. Obtained equilibrium data were then fitted to different competitive multicomponent isotherm models like Langmuir (extended), Freundlich isotherm (extended), Sheindrof‐Rebuhn‐Sheintuch (SRS) isotherm and Redlich‐Peterson isotherm (modified) models, and various isotherm interaction parameters were calculated.