Exchange bias (EB) presents the interfacial coupling between ferromagnetic (FM) and antiferromagnetic (AFM) phases, which could be applied for high-density data storage and magnetic recording. In thin films, the EB effect could be realized in either a FM/ AFM multilayer structure or a FM/AFM vertically aligned nanocomposite (VAN) form, which allows the interfacial coupling tuning along the horizontal or perpendicular directions, respectively. Here, to combine the schemes of multilayer and VAN structures, a new 3D nanocomposite has been designed, which is La 0.7 Sr 0.3 MnO 3 (LSMO)/NiO VAN layers with inserted LSMO or NiO layers. Such a 3D nanocomposite structure provides a great platform to tailor the EB effect along both horizontal and perpendicular directions. Specifically, the sample with a NiO interlayer exhibits the highest EB field (H EB ) of 350 Oe and 475 Oe under in-plane and out-of-plane field, respectively. Furthermore, the H EB value and Curie temperature (T c ) can be tuned by different 3D nanostructures. This work demonstrates the double EB modulation with the designed 3D nanostructures as a new route toward advanced magnetic data storage and spintronic devices.