Organometallic conjugated complexes have become an important type of stimuli-responsive materials because of their appealing electrochemical properties and rich photonic, electronic, and magnetic properties. They are potentially useful in a wide range of applications such as molecular wires, molecular switches, molecular machines, molecular memory, and optoelectronic detections. This review outlines the recent progress on the molecular design of carbometalated ruthenium and osmium complexes and their applications as redox-responsive materials with visible and near-infrared(NIR) absorptions and electron paramagnetic resonance as readout signals. Three molecule systems are introduced, including the symmetric diruthenium complexes, metal-amine conjugated bi-center system, and multi-center redox-active organometallic compounds. Because of the presence of a metal-carbon bond on each metal component and strong electronic coupling between redox sites, these compounds display multiple reversible redox processes at low potentials and each redox state possesses significantly different physical and chemical properties. Using electrochemical potentials as input signals, these materials show reversible NIR absorption spectral changes, making them potentially useful in NIR electrochromism and information storage. Organometallic conjugated complexes have become an important type of stimuli-responsive materials because of their appealing electrochemical properties and rich photonic, electronic, and magnetic properties. They are potentially useful in a wide range of applications such as molecular wires, molecular switches, molecular machines, molecular memory, and optoelectronic detections. This review outlines the recent progress on the molecular design of carbometalated ruthenium and osmium complexes and their applications as redox-responsive materials with visible and near-infrared (NIR) absorptions and electron paramagnetic resonance as readout signals. Three molecule systems are introduced, including the symmetric diruthenium complexes, metal-amine conjugated bi-center system, and multi-center redox-active organometallic compounds. Because of the presence of a metal-carbon bond on each metal component and strong electronic coupling between redox sites, these compounds display multiple reversib le redox processes at low potentials and each redox state possesses significantly different physical and chemical properties. Using electrochemical potentials as input signals, these materials show reversible NIR absorption spectral changes, making them potentially useful in NIR electrochromism and information storage.