<p>Anode-free all-solid-state batteries (AFSSBs) have recently gained increasing interest due to their simplified cell configuration and reduced inactive components, as lithium is plated directly onto the current collector. However, challenges such as unstable lithium nucleation and interfacial incompatibility between the solid electrolyte and current collector continue to limit their practical development. In this study, a freestanding carbon nanotube (CNT) film interlayer was introduced to promote more uniform lithium-ion transport and to buffer interfacial volume variations during repeated plating and stripping. To address the intrinsically low lithiophilicity of CNT film, silver (Ag) nanoparticles were uniformly anchored onto the surface via a surfactant-assisted wet-chemical process conducted under ambient conditions. This approach offers a relatively simple and scalable route for interlayer modification without the need for vacuum or high-temperature treatments. The incorporation of Ag reduced lithium nucleation overpotential and decreased the charge-transfer resistance, contributing to more homogeneous lithium deposition behavior. At a current density of 1.167&#xa0;mA&#xa0;cm⁻² and areal capacity of 3.5&#xa0;mAh&#xa0;cm⁻², the modified interlayer maintained a Coulombic efficiency of 96.68% at room temperature. These findings suggest that the Ag–CNT interlayer can effectively improve interfacial characteristics and lithium nucleation behavior in AFSSBs, offering insight into interfacial design strategies for high-energy–density solid-state batteries.</p> Graphical Abstract <p></p>