Recently, three-dimensional (3D) electrode architectures have attracted great interest for the development of lithium-ion micro-batteries applicable for Micro-Electro-Mechanical Systems (MEMS), sensors, and hearing aids. Since commercial available micro-batteries are mainly limited in overall cell capacity by their electrode footprint, new processing strategies for increasing both capacity and electrochemical performance have to be developed. In case of such standard microbatteries, two-dimensional (2D) electrode arrangements are applied with thicknesses up to 200 μm. These electrode layers are composed of active material, conductive agent, graphite, and polymeric binder. Nevertheless, with respect to the type of active material, the active material to conductive agent ratio, and the film thickness, such thick-films suffer from low ionic and electronic conductivities, poor electrolyte accessibility, and finally, limited electrochemical performance under challenging conditions. In order to overcome these drawbacks, 3D electrode arrangements are under intense investigation since they allow the reduction of lithium-ion diffusion pathways in between inter-digitated electrodes, even for electrodes with enhanced mass loadings. In this paper, we present how to combine laser-printing and femtosecond laser-structuring for the development of advanced 3D electrodes composed of Li(Ni1/3Mn1/3Co1/3)O2 (NMC). In a first step, NMC thick-films were laser-printed and calendered to achieve film thicknesses in the range of 50 μm – 80 μm. In a second step, femtosecond laser-structuring was carried out in order to generate 3D architectures directly into thick-films. Finally, electrochemical cycling of laser-processed films was performed in order to evaluate the most promising 3D electrode designs suitable for application in long life-time 3D micro-batteries.