to photodynamic therapy (PDT), [12][13][14][15][16][17][18] drug delivery, [19][20][21][22][23][24][25][26] molecular detection, [27][28][29][30][31] optogenetics, [32][33][34] etc. On the other side, broader applications of UCNPs are hindered by their low extinction coefficients and quantum efficiency as well as fixed energy levels. [1,[35][36] Moreover, various energy transfer paths among these lanthanide cations often result in deleterious cross-relaxations. Thus, specific multiplexed applications require compositional and structural UCNPs design to be delicate and complex. The creation of such structures is multi-step and timeconsuming. [7,19,[37][38][39][40][41] To resolve these problems, scientists tried to develop UCNPs assemblies containing various UCNPs or UCNPs and other functional counterparts. The resulting composites exhibited unique properties, determined by the dimension and morphology of the individual components and the whole assembly. These properties can also be tuned depending upon the application situation such as dual-modality cell imaging, [26,[42][43] drug delivery, [44][45][46][47][48][49] molecular detection, [50][51] and programmed control therapy. [47][48] In terms of multifunctionality, the UCNPs assembly not only preserve the original upconverting characteristics of UCNPs but also endowed with variable other functional properties with much improved. All these properties help to improve performance and overcome the limitations of UCNPs. The composition, morphology, and assembly manner of individual components can be tuned to obtain the desired properties and adjust them to the specific environment when needed. Combining UCNPs with other materials (quantum dots, [43] metals, [51] polymers, [52][53] DNA, [26,42,54] etc.) minimizes the challenges connected to the UCNPs implementation allowing the resulting materials to exhibit multifunctionalities. These approaches made the composites containing UCNPs very promising for a variety of applications.Recently, a variety of UCNPs assembly synthesis methods was developed, which involve interface, [55][56][57] microemulsion, [52,[58][59] and polymer/DNA [26,46,60] meditated method. Meanwhile, it is not hard for us to observe the appearance of UCNPs assembly in some new applied fields such as DNA detection, [50][51] chemo-photodynamic therapy, [53,60] and programmable therapeutics. [45,[47][48] A grasp of the achievements on the UCNPs assembilies reported over the last years would assist scientists to fully utilize the UCNPs based nanoplatforms for various applications. Thus, Section 2 of this review describes UCNPs properties, and Sections 3 is dedicated to UCNPsIn the past few decades, significant progress of the conventional upconversion nanoparticles (UCNPs) based nanoplatform has been achieved in many fields, and with the development of nanoscience and nanotechnology, more and more complex situations need a UCNPs based nanoplatform having multifunctions for specific multimodal or multiplexed applications. Through self-assembly, different UCN...