Demolding is a crucial step in nanoimprint lithography (NIL) for successfully transferring template structures onto resist materials. The process, however, is often hindered by the adhesion and friction between the template and resist, leading to inevitable defects on the replicas and posing challenges in replicating templates with high-aspect-ratio (HAR) structures. Here, we introduce a novel approach using the dissolvable template method to achieve the nondestructive demolding of structure-designable HAR nanoimprint templates. The templates were fabricated by the 3D lithography technology, employing a positive photoresist that can be easily dissolved in alkaline solutions after exposure to ultraviolet (UV) radiation. By implementing this method, we successfully transferred dense arrays of pillars with a minimal diameter of 1.2 μm and a significant aspect ratio of 18, as well as a microlens array diffuser with randomly distributed structural parameters. The dissolvable template method paves the way for stress-free demolding, broadening NIL’s application range.