Electrical conductivity, mechanical flexibility, and large electroactive surface areas are the most important factors in determining the performance of various flexible electrodes in energy storage devices. Herein, a layer‐by‐layer (LbL) assembly‐induced metal electrodeposition approach is introduced to prepare a variety of highly porous 3D‐current collectors with high flexibility, metallic conductivity, and large surface area. In this study, a few metal nanoparticle (NP) layers are LbL‐assembled onto insulating paper for the preparation of conductive paper. Subsequent Ni electroplating of the metal NP‐coated substrates reduces the sheet resistance from ≈103 to <0.1 Ω sq−1 while maintaining the porous structure of the pristine paper. Particularly, this approach is completely compatible with commercial electroplating processes, and thus can be directly extended to electroplating applications using a variety of other metals in addition to Ni. After depositing high‐energy MnO NPs onto Ni‐electroplated papers, the areal capacitance increases from 68 to 811 mF cm−2 as the mass loading of MnO NPs increases from 0.16 to 4.31 mg cm−2. When metal NPs are periodically LbL‐assembled with the MnO NPs, the areal capacitance increases to 1710 mF cm−2.