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Er3+/Yb3+-codoped NaLa(MoO4)2 colloidal nanocrystals were synthesized by pulsed laser ablations in de-ionized water andsodium dodecyl sulfate (NaC12H25SO4, SDS) aqueous solution for up-conversion (UC) luminescence bio-labeling applications. The influences of the SDS molecules on the crystallinities, crystal morphologies, crystallite sizes, and UC luminescence propertiesof the prepared Er3+/Yb3+-codoped NaLa(MoO4)2 colloidal nanocrystals were investigated in detail. Under a 980-nm excitation,the Er3+/Yb3+-codoped nanocolloidal NaLa(MoO4)2 suspension exhibited a weak red emission near 670 nm and strong green UCemissions at 530 and 550 nm, corresponding to the intra 4f transitions of Er3+ (4F9/2, 2H11/2 , 4S3/2)→Er3+ (4I15/2). When the SDSsolution was used, a smaller average crystallite size, narrower size distribution, and enhanced UC luminescence were observed. These characteristics were attributed to the amphoteric SDS molecules attached to the positively charged Er3+/Yb3+-codopedNaLa(MoO4)2 colloidal nanocrystals, effectively occupying the oxygen defect on their surfaces. The Er3+/Yb3+-codopednanocrystalline NaLa(MoO4)2 suspension prepared in the SDS solution exhibited a remarkably strong green emission visibleto the naked eyes.