AbstractHere, the 3D‐printing of supramolecular polymer electrolytes is reported, able to be manufactured via 3D‐printing processes, additionally dynamically compensating for volume changes. A careful mechanical design, in addition to rheological effects observed for different additives to the electrolyte, is investigated and adjusted, in order to achieve printability via an extrusion process to generate a conductive electrode material. Qudruple‐hydrogen bonds (UPy) act as supramolecular entities for the desired dynamic properties to adjust printability, in addition to added LiTFSi‐salts to achieve ionic conductivities of ≈10–4 S cm–1 at T = 80 °C. Three different telechelic UPy‐PEO/PPO‐UPy‐polymers with molecular weights ranging from Mn = 600–1500 g mol−1 were investigated in view of their 3D‐printability by FDM‐processes. It is found that there are three effects counterbalancing the rheological properties of the polymers: besides temperatures, which can be used as a known tool to adjust melt‐rheology, also the addition of lithium‐salts in junction with the polymers crystallinity exerts a major toolbox to 3D‐print these electrolytes. Using specific compositions with Li/EO‐ratios from 20:1, 10:1, and 5:1, the rheological profile can be adjusted to reach the required printability window. AT‐IR‐investigations clearly indicate a weakening of the UPy‐bonds by the added Li+ ions, in addition to a reduction of the crystallinity of the PEO‐units, further changing the rheological profile. The so generated electrolytes are printable systems for novel electrolytes.