In this paper, we synthesized ~105±15 nm cubic phase KMnF3:Yb3+,Er3+ NPs, ~195±10 nm hexagonal phase NaYF4:Yb3+,Tm3+ NPs, and ~200±10 nm hexagonal phase NaYF4:Yb3+,Er3+ NPs. Under the excitation of 980 nm, the strong red upconversion luminescence (4F9/2⟶4I15/2, the peak is located at ~653 nm) of Er3+ ions of KMnF3:Yb3+,Er3+ NPs can be seen, the strong blue upconversion luminescence (1D2⟶3F4, 1G4⟶3H6; the peaks are located at ~451 nm and ~477 nm, respectively) of Tm3+ ions of NaYF4:Yb3+,Tm3+ NPs can be observed, and the strong green upconversion luminescence (4I11/2⟶4I15/2, 4S3/2⟶4I15/2; the peaks are located at ~524 nm and ~541 nm, respectively) of Er3+ ions of NaYF4:Yb3+,Er3+ NPs can be found. The mixed white upconversion luminescent materials can be obtained by adjusting the doping ratio of the above NPs. Cyclohexane solution of red, blue, green, and the mixed white NPs can be used as ink, and “JLNU” is written on paper with a pen. Without 980 nm radiation, nothing could be seen. Under 980 nm irradiation, the colored letters “JLNU” can be seen. Red, blue, green, and the mixed white upconversion NPs can be used in security anticounterfeiting.