In this study, we investigate the strategic spatial integration of a conducting polymer into lithium electrodes for energy storage applications. Poly(3,4-ethylenedioxythiophene) (PEDOT) was incorporated into 2D graphene-molybdenum disulfide (GM) heterolayers to enhance their electrochemical performance in lithium-ion hybrid capacitors (LHCs). Two design strategies were explored: (i) N-PGM with an intra-embedded 3D PEDOT network via vapor-phase polymerization (VDP), and (ii) L-PGM with an outer 2D PEDOT layer deposited in the final fabrication step. N-PGM exhibited improved rate capability over GM, while L-PGM achieved the highest specific capacity and excellent cycling stability, retaining over 95.3% of its capacity after 2000 cycles. PEDOT introduced an additional surface-driven charge storage mechanism, complementing the diffusion-limited redox behavior of MoS₂. Molecular dynamics simulations further revealed that PEDOT weakened direct Li⁺ binding but improved electrolyte compatibility and ion mobility. Notably, the spatial configuration of PEDOT critically influenced these effects: surface-localized PEDOT in L-PGM reduced Li⁺ adsorption energy and promoted faster ion diffusion, whereas embedded PEDOT in N-PGM maintained a balance between ion transport and retention. These findings highlight that spatially controlled polymer incorporation offers a promising route to optimizing ionic accessibility and charge transport in nanostructured electrodes.

Conventional approaches to perovskite superlattice (SL) synthesis typically involve multi‐step processing with post‐synthetic treatments, which often suffer from limited control, poor reproducibility, and scalability issues. Herein, we report a one‐step solution‐phase protocol for the synthesis of structurally stable, 3D CsPbBr ₃ nanocrystal SLs using an amphiphilic double‐tailed ligand (cesium bis(2‐ethylhexyl) sulfosuccinate, Cs‐AOT) in combination with conventional ligands, and precisely controlled amounts of water. This approach enables rapid, spontaneous, and highly uniform SL assembly directly in solution within seconds, without any additional post‐processing. Systematic investigations reveal that isotropic nanocrystal growth and ordered SL formation critically depend on the interplay between ligand–ligand interactions, nanoconfined water, and reverse micelle formation. Molecular dynamics simulations and structural analyses further show that water migration enhances ligand mobility through polarity compensation, thereby strengthening interparticle entanglement and stabilizing the SLs in solution. The as‐synthesized CsPbBr ₃ SLs demonstrate exceptional structural stability and enhanced emission properties, thereby enabling practical applications such as high‐performance anti‐counterfeiting optical quick response codes. This work provides fundamental insights into ligand–water interactions governing perovskite SL assembly and offers a scalable synthetic pathway for advanced functional SL materials.

Conducting polymers (CPs) have emerged as multifunctional components that modulate electrolyte and separator design for Zn-ion hybrid capacitors, with selected Zn-based battery and alkali-ion systems used as mechanistic references rather than direct performance evidence. Their π-conjugated backbones, tunable doping states, and reversible redox chemistry enable coupled ion transport, interfacial charge regulation, and mechanically compliant ion-conducting environments. However, CP integration also requires careful control of electronic leakage, self-discharge, short-circuit risk, and redox-state-dependent swelling, particularly when CP domains are introduced into separator architectures. This review examines how CP-containing electrolytes and separator-related architectures can regulate ion transport and interfacial charge distribution, provided that continuous electronic pathways are suppressed. In aqueous, quasi-solid gel, solid polymer, and redox-active electrolytes, CP-containing domains are examined in terms of ionic conductivity, Zn²⁺ transport, solvation regulation, and polarization mitigation. In separator-related architectures, spatially confined and electronically interrupted CP domains are discussed with emphasis on ion-flux homogenization, dendrite suppression, electron-blocking requirements, and dimensional stability. Comparative analyses separate directly demonstrated Zn-ion hybrid capacitor behavior from mechanisms inferred from related ion-storage systems. Finally, future directions are discussed for quantitative benchmarking, scalable CP processing, and architecture-controlled CP domains for coordinated electrolyte and separator design.