This study focuses on the design, fabrication, and characterization of deterministically engineered, three-dimensional architectures to be used as high-performance electrodes in energy storage applications. These high-surface-area architectures are created by the robotically-assisted sequential electrodeposition of structural and sacrificial layers in an alternating fashion, followed by the removal of the sacrificial layers. The primary goal of this study is the incorporation of these highly laminated architectures into the battery electrodes to improve their power density without compromising their energy density. MEMS technologies, as well as electrochemical techniques, are utilized for the realization of these high-power electrodes with precisely controlled characteristic dimensions. Diffusion-limited models are adopted for the determination of the optimum characteristic dimensions of the electrodes, including the surface area, the thickness of the active material film, and the distance between the adjacent layers of the multilayer structure. The contribution of the resultant structures to the power performance is first demonstrated by a proof-of-concept Zn-air microbattery which is based on a multilayer Ni backbone coated with a conformal Zn film serving as the anode. This primary battery system demonstrates superior performance to its thin-film counterpart in terms of the energy density at high discharge rates. Another demonstration involves secondary battery chemistries, including Ni(OH)2 and Li-ion systems, both of which exhibit significant cycling stability and remarkable power capability by delivering more than 50% of their capacities after ultra-fast charge rates of 60 C. Areal capacities as high as 5.1 mAh cm-2 are reported. This multilayer fabrication approach is also proven successful for realizing high-performance electrochemical capacitors. Ni(OH)2-based electrochemical capacitors feature a relatively high areal capacitance of 1319 mF cm-2 and an outstanding cycling stability with a 94% capacity retention after more than 1000 cycles. The improved power performance of the electrodes is realized by the simultaneous minimization of the internal resistances encountered during the transport of the ionic and electronic species at high charge and discharge rates. The high surface area provided by the highly laminated backbone structures enables an increased number of active sites for the redox reactions. The formation of a thin and conformal active material film on this high surface area structure renders a reduced ionic diffusion and electronic conduction path length, mitigating the power-limiting effect of the active materials with low conductivities. Also, the highly conductive backbone serving as a mechanically stable and electrochemically inert current collector features minimized transport resistance for the electrons. Finally, the highly scalable nature of the multilayer structures enables the realization of high-performance electrodes for a wide range of applications from autonomous microsystems to macroscale portable electronic devices.