Multicolor luminescent nanoparticles (NPs) show several potential emerging applications. In this work, we provide a new route that integrates the afterglow and upconversion (UC) that originate in a single activator to achieve color variations without the modulation of any other parameters. The Er3+ ions in Na3HfF7:Yb/Er NPs exhibit bright green afterglow upon X-ray irradiation and single-band red UC under 980 nm laser excitation, which are attributed to the significantly different electron population pathways. The UC intensity is stable and the afterglow decreases gradually over time, thus the output color is clearly changed from green to red naturally via illuminating the pre-X-ray-irradiated NPs with a 980 nm laser. Furthermore, the fine emission profiles of Er3+, Ho3+ and Tm3+ are achieved upon X-ray irradiation. Our results develop a new approach for time-dependent dynamic color displays and a simple route to revealing the electronic fine structures of lanthanide activators at room temperature.