Digital light processing (DLP)-based three-dimensional (3D) printing is an ideal tool to manufacture hydrogel structures in complex 3D forms. Using DLP to print hydrogel structures with high resolution requires the addition of water-soluble photo-absorbers to absorb excess light and confine photopolymerization to the desired area. However, the current photo-absorbers for hydrogel printing are neither efficient to absorb the excess light nor water-soluble. Herein, we report a volatile microemulsion template method that converts a wide range of commercial non-water-soluble photo-absorbers including Sudan orange G, quercetin, and many others to water-soluble nanoparticles with solubility above 1.0 g mL-1. After using these water-soluble photo-absorber nanoparticles, the highest lateral and vertical resolutions of printing high-water-content (70-80 wt%) hydrogels can be improved to 5 μm and 20 μm, respectively. Moreover, the quercetin nanoparticle can be easily washed out so that we achieve colorless and transparent printed hydrogel structures with excellent mechanical deformability and biocompatibility as well as thermally controllable variations on transparency and actuation. The proposed methods pave a new efficient way to develop water-soluble photo-absorbers, which helps to greatly improve the printing resolution of the high-water-content hydrogel structure and would be beneficial to extend the application scope of hydrogels.