An environment-friendly fluorescent nano-hybrid hydrogel has been synthesized successfully, from cellulose nanocrystal (CNC), acrylic acid (AA) and phosphorescent Eu2+/Dy3+ doped SrAl2O4 via free radical polymerization. The hydrogel network matrix fixed Eu2+/Dy3+ doped SrAl2O4 nanoparticles by polymer chains with coordinate bonds that prevented particles from aggregating and quenching in water. The fluorescent nano-hybrid hydrogel exhibited extremely high water absorption of which the swelling ratio in distilled water and NaCl salt solution were respectively of 323.35 g/g and 32.65 g/g. Furthermore, the hydrogel displayed excellent water retention property that can keep half of the moisture even exposed to 80 °C for 210 min. Besides, the hydrogel had bright green fluorescence under the sunlight or ultraviolet excitation, and the fluorescence intensity was up to 125477 after swelling 50 times in water. The time-resolved photoluminescence (TRPL) afterglow decay examination showed that the fluorescent emission persisted for 4 h after hydrogels excited at 368 nm wavelength UV-light for 10 min. The fluorescence intensity behaved significant linear relationship with the swelling ratio. As a result, these hydrogels were considered as promising candidates for the preparation of stable and sensitive sensor materials in green water detection.