β-NaYF 4 UCMPs are large-scale synthesized, and the UCMPs fluorescence inks-based screen printing patterns are applied for anti-counterfeit application.Abstract: Upconversion materials could be applied for anti-counterfeit fields because of their high concealment and high upconversion fluorescence efficiency. Herein, the different lanthanide ions-doped β-NaYF 4 upconversion micro-particles (UCMPs) with uniform hexagonal morphology were large-scale synthesized (more than 0.5 g) through a facile hydrothermal method. It is very interesting to find out the fluorescence intensity and the eventual morphology of UCMPs are highly dependent on the reaction conditions. Then, the optimal UCMPs with uniform morphology and strong fluorescence intensity were selected as promising candidate for preparing ink.Eventually, we successfully printed designable and multicolor fluorescent patterns on flexible substrates (common paper and polyethylene terephthalate, PET) by using the as-prepared β-NaYF 4 : Yb 3+ , Tm 3+ /Er 3+ /Eu 3+ UCMPs inks. Under ambient conditions, the printed patterns on conventional paper are invisible, while such printed patterns on PET are white color. But all the patterns could perform blue, yellow-green and green fluorescence patterns under the irradiation of 980 nm lasers, respectively, when using β-NaYF 4 : Yb 3+ , Tm 3+ /Er 3+ /Eu 3+ UCMPs inks. We envision that the UCMPs fluorescent inks-based flexible and rapid screen printing patterns have an enormous potential for anti-counterfeit and security applications.