Imprinting is a well-established technique to induce recognition features in both organic and inorganic materials for a variety of target analytes. In this study, ion imprinted polysiloxanes with varying percentage of coupling agent i.e. 3-chloro propyl trimethoxy silane (CPTM) were synthesized by sol-gel method for imprinting of Cr3+. The imprinting of Cr3+ in cross-linked siloxane network was investigated by FT-IR which indicates the metal ion is coordinated with oxygen atoms of polysiloxanes. SEM images revealed that imprinted polysiloxanes possess uniform particles of submicron size. It was experienced that by increasing the concentration of CPTM up to 10% (v/v) substantially improves the binding capacity of polysiloxanes which allows us to recognized Cr3+ down to 50µg/L. Furthermore, the selectivity of Cr3+-imprinted polysiloxanes was evaluated by treating them with other competing metal ions of same concentration i.e. Cr6+, Pb2+ and Ni2+. In this regard, polysiloxanes showed much higher binding for imprint ion i.e. Cr3+ in comparison to above mentioned metal ions. Finally, the regenerated polysiloxanes were studied in order to reuse them thus, developing cost effective biomimetic sensor coatings.