A lot of every day devices are electrically powered and dependent on an internal energy source. One of the most used energy sources for portable devices are rechargeable batteries. Throughout the last decades, battery research and development gave rise to significant performance improvements. New electrode materials, design strategies and advanced fabrication techniques have equipped modern-day batteries with ever-rising capacity. However, little changed in their appearance, shape, and functionalities. On the other hand, development of flexible devices stays on the horizon. Without adequate evolution of the energy storage unit, development of those devices is severely hampered. Powering flexible devices requires flexible, mechanically strong and lightweight energy storage units. In contrary, commercial batteries are mechanically susceptible to external stresses from bending, highlighting the current hurdle of powering flexible devices with commercial batteries. High-capacity materials, namely metal and alloying anodes, as well as conversion cathodes would make cells and devices lighter and smaller. However, these materials currently possess unsolved challenges in material integrity and cycling stability. Adding bending stresses in flexible devices make the battery even more vulnerable to capacity decay. All in all, this leads to a distinguished trade-off between batteries with high capacity and ones with good bending stability. This thesis aims to tackle the challenge by investigating and optimizing the compatibility of high-capacity electrode materials with a flexible substrate. The work shows that carbon-based materials provide a versatile, conductive platform to stabilize and utilize high-capacity materials in flexible devices, demonstrated with two battery chemistries – namely zinc-ion and lithium-sulfur batteries. Carbon materials are introduced as a lightweight conductive platform to process stiff, brittle and/or powdery electrode materials into structures that are flexible. A conductive network is formed via self-assembly of single-walled carbon nanotubes (CNT) upon drying. Their bending stability could be verified even upon integration of 40 wt% active material. In particular, high aspect ratio CNTs formed flexible substrates with incorporated materials for silicon anode and sulfur cathode in lithium-sulfur cells. Accordingly, silicon-gallium composite with Page | III chitosan-alginate binder and sulfur with nitrogen-doped titanium oxide integrated into CNT network exhibited stable electrochemical performance in half-cells. Furthermore, the preparation method was adapted to the respective active materials for zinc-ion batteries in a Zn-MnO2 cell and has the potential to incorporate various other active materials. One approach to flexibility relies on thinning down the material layers. However, among the challenges in thin batteries, dendrite formation and their control of metal anodes is one of the crucial factors to maintain the cell performance. Dendrite growth mechanism is unique to the respective metal surface and interacting battery components. Zinc and its cycling behaviour were studied as one of the battery systems with decent capacity, but prone to dendrite formation. Without mitigation measures, zinc surfaces form dendrites under stripping and plating in near neutral electrolyte, which leads to short circuit. This thesis demonstrates a functionalization process on zinc anodes by simple surface assembled monolayer of thiols. The additives improve the cycle of short circuit at 1 mAh/cm2, one order of magnitude compared to pristine zinc surfaces. Intrinsic electrochemical and mechanical stability, together with interfacial adhesion, define the robustness of a flexible battery. With the CNT network proven to show compatibility with two, rather different battery chemistries, it can be assumed that further investigations will show universal application of this carbon-based material as substrate for flexible electrode fabrication. Furthermore, the investigations on different aspects of stability in high-capacity active materials show progress towards better cycling stability of materials in zinc and lithium batteries. Light, thin and flexible electrochemical energy storage devices meet the criteria of the fast-evolving fields of wearable sensing devices and rollable personal electronics. New functionalities of electrochemical cells potentially create new integration opportunities or even facilitate completely new applications. This research paves the way toward developing flexible devices and digitalization in everyday life.