The tailoring of smart material properties is one of the challenges in materials science. The unique features of polymers with pendant ferrocene units, either as ferrocenyl or ferrocenediyl groups, provide electrochemical, electronic, optoelectronic, catalytic, and biological properties with potential for applications as smart materials. The possibility to tune or to switch the properties of such materials relies mostly on the redox activity of the ferrocene/ferricenium couple. By switching the redox state of ferrocenyl units - separately or in a cooperative fashion - charge, polarity, color (UV-vis range) and hydrophilicity of polymers, polymer functionalized surfaces and polymer derived networks (sol-gel) may be controlled. In turn, also the vicinity of such polymers influences the redox behavior of the pendant ferrocenyl units allowing for sensing applications by using polymer bound enzymes as triggering units. In this review the focus is set mainly on the literature of the past five years.