The dopant concentration of lanthanide ions plays one of the critical roles to manipulate size/morphology, photon population pathway, or luminescence color/intensity in upconversion nanoparticles (UCNCs), which have a significant effect on their application developments. Herein, a strategy is demonstrated for simultaneous size, morphology and multicolor luminescence tuning in the single doped lanthanide activator Er3+ ion system through simply tuning the concentration of Er3+ ions. The doping of different Er3+ ion amounts in NaYbF4:Er nanocrystals can control nanoparticle size (from several hundreds to tens of nanometers) and morphology. Moreover, multicolor upconversion luminescence involving green, yellow, orange and red can be obtained in the NaYbF4:Er UCNCs by changing the excitation power density of 980 nm laser. Mechanistic studies reveal the size and morphology evolution process as well as saturation/cross relaxation effects induced tunable multicolor emissions. These nanocrystals have demonstrated promising potential applications in anticounterfeiting. Our results not only provide a simple and feasible route for simultaneous size/morphology control and multicolor upconversion luminescence tuning, but also can further expand the utility of UCNCs in the frontier applications ranging from optical encoding to information security.