Structural DNA nanotechnology has emerged as a versatile tool to build elaborate nanostructures in a convenient, biocompatible and user-friendly way. By exploiting specific DNA base-pairing principles, it is now possible to program the assembly of cocktails of synthetic DNA strands into virtually any desired 2D or 3D morphologies. The resulting structures are not only obtained at a high yield with great precision, but they can also be used as universal scaffolds to spatially organize bound entities (proteins, particles, etc.) with subnanometric resolution, leading to a vast range of applications, from materials science to biomedicine. The underlying DNA self-assembly principles impose however some limits. First, most approaches rely on the use of a scaffold, as in the case of DNA origamis, which strongly limits the size of the final self-assembled structures, typically up to around 100 nm, unless specific additional protocols are applied. Additionally, despite the recent development of isothermal DNA self-assembly principles, the vast majority of methods rely on a thermal annealing step to ensure flawless assembly between the multitude of DNA strands. This temperature treatment, consisting in heating the system above the melting temperature before a slow cooling down ramp, takes usually hours to days, thus imposing strong temporal constraints on the assembly. To expand the potential offered by programmable DNA self-assembly, it would be highly valuable to identify principles orthogonal to basepairing rules, in which DNA nanostructures could be assembled into well-defined superstructures, both extended in space and produced in a rapid manner. We suggest to approach such a goal by getting inspired by the fact that, in nature, DNA is usually present in a variety of higher-ordered structures not solely relying on Watson-Crick-Franklin interactions. For instance, genomic DNA of viruses, eukaryotes and prokaryotes are highly organized thanks to a combination of interactions where electrostatics plays a major role. It has been shown in particular that double-stranded DNA, which adopts an elongated coil conformation in water due to the strong electrostatic repulsions between the phosphate groups along its backbone, undergoes a dramatic transition into highly ordered structures, such as toroids, when small multivalent cations, including naturally occurring polyamines such as spermidine and spermine, are added. We envisaged that this principle could be used to rapidly reorganize self-assembled DNA nanostructures into higher-order superstructures. The exploitation of electrostatic interactions for such a purpose has already been explored but only in a few notable cases. In the case of DNA origamis, solid substrates were used to generate electrostatically tunable lattices or induce intramolecular suprafolding transition in the case of soft cationic polymer layer. The requirement of solid substrates limits however the versatility and applicability of the resulting assemblies. In bulk, intramolecular reconfiguration upon addition of positively charged proteins and intermolecular assemblies mediated by cationic nanoparticles were reported. However, DNA origamis, remaining small building blocks, are not well suited for the construction of extended 3D assemblies. For their elongated geometry and possibility to reach micrometric dimensions, DNA nanotubes obtained by the self-assembly of single-stranded or double-crossover tiles, appear as more promising starting materials. For instance, the addition of crowding agents or magnesium ions induced the formation of asters or bundles, respectively, while specifically designed macromolecular star-shaped cationic crosslinking agents led to contractile rings. Surprisingly, the use of naturally occurring polyamines for the assembly of DNA nanotubes has never been explored. Moreover, although DNA condensation is a reversible process, the possibility of dynamically disassembling DNA nanotubes superstructures has been overlooked. Here, we used a simple cocktail of 5 DNA strands leading to long self-assembled nanotubes and studied how they reorganized upon addition of two naturally occurring polyamines known as DNA condensing agents, the triamine spermidine (noted SPD 3+ ) and the tetraamine spermine (noted SPM 4+ ), and compared with the effect of magnesium ion (Mg 2+ ). Using fluorescence and electron microscopy, we revealed the reproducible formation of a diversity of superstructures, including bundles, rings as well as novel organizations into extended networks. We established phase diagrams highlighting the importance of counter-ion valency rather than specific interactions and proposed methods to reversibly disassemble the superstructures into nanotubes through monovalent salt addition. We also explored the possibility of photocontrolling the superstructure formation in the presence of a photosensitive DNA condensing agent.