Organic materials for Li-ion battery application continue gaining attention due the virtue of low cost, environmental benignity, and so on. A new class of electroactive organic material called polyimides is particularly important due to the extra stability exhibited at higher current rates. High-performance rechargeable lithium battery cathodes based on polyimides of 3,4,9,10-perylenetetracarboxylicacid-dianhydride are prepared. The novel electrodes exhibit good rate capability and improved cycling stability, which result from their combined beneficial properties such as the presence of additional carbonyl groups, favorable band gap, and enhanced conductivity, making it a potential material for greener and sustainable electrochemical storage devices. SECTION: Energy Conversion and Storage; Energy and Charge Transport S torage and utilization of sustainable energy via an environmentally friendly route is an important aspect of energy economy. 1−3 With a growing need for clean and efficient energy-storage technologies, rechargeable Li-ion batteries are undoubtedly the state-of-the-art and hence continue to gain both scientific and commercial importance for their applications in portable electronics and vehicular sector. 4−6 However, designing advanced batteries that are highly energy efficient and eco-friendly is still a major challenge. The current Li-ion battery technology with active inorganic insertion electrode materials such as LiCoO 2 fails to fulfill the demand in terms of safety and sustainability. Recently, there has been wide interest toward developing "greener and sustainable" rechargeable lithium batteries based on organic electrode-active materials. 7−10 Research on organic electrodes for rechargeable lithium batteries, although started several years back, did not gain much importance until recently, partially due to their poor performances and wide acceptance of transitional-metal-based inorganic electrodes. Transition from inorganic to organic material-based electrodes could be a possible alternative, and several groups have turned toward "organic approach", thanks to the rich and versatile chemistry available for organic synthesis that allows the design of electrode materials with high level of control over the functionalities and tunable redox properties without the use of heavy metals and hightemperature synthesis. 1 In recent years, several redox-active organic materials such as organosulphur, 11 radical polymers, 12,13 and carbonyl 14 -based compounds have been studied as electrodes for Li-based batteries and were reported to exhibit reversible reactivity with Li. However, the performance characteristics of such organic electrodes for their application in Li-ion battery were limited due to several factors such as electrode dissolution, thermal instability, and so on. Reversible redox properties of carbonyl-based organic molecules have been extensively studied by several groups. 1,10,14−16 Nevertheless, organic-based materials present some drawbacks such as low thermal stability, low conductivit...