It remains challenging to fabricate Tb 3+ -doped lanthanide nanocrystals (NCs) for acquiring strong energy migration upconversion (EMU) emissions of Tb 3+ , while simultaneouly suppressing the Tm 3+ ultraviolet upconversion emissions that cause the issue of background biofluorescence in bioapplications based on Tb 3+doped EMU NCs. Herein, we report a novel sandwich structure core@shell@shell scheme for the design of EMU NCs, e.g. NaLuF 4 :Yb/Gd@NaGdF 4 :Tm@NaLuF 4 :Tb NCs, wherein Yb 3+ , Tm 3+ , and Tb 3+ are separately incorporated into the inner core, middle shell, and outer shell, respectively. We have found that, in the sandwich structure NCs, the effective inter-shell energy transfer from Gd 3+ in the middle shell to Tb 3+ in the outer shell accelerates the Yb 3+ -Tm 3+ five-photon upconversion and subsequent Tm 3+ to Gd 3+ energy transfer processes, which can eventually lead to the nearly completely inhibited Tm 3+ ultraviolet upconversion emissions concomitant with the strong EMU emissions of Tb 3+ . Our findings might stimulate new concepts for manipulating upconversion emissions of lanthanide NCs.