Upconversion is a nonlinear optical phenomenon that involves the emission of high‐energy photons by sequential absorption of two or more low‐energy excitation photons. Due to their excellent physiochemical properties such as deep penetration depth, little damage to samples, and high chemical stability, upconversion nanoparticles (UCNPs) are extensively applied in bioimaging, biosensing, theranostic, and photochemical reactions. Here, recent achievements in the synthesis, optimization, and applications of UCNP‐based nanomaterials are reviewed. The state‐of‐the‐art approaches to synthesize UCNPs in the past few years are introduced first, followed by a summary of several strategies to optimize upconversion emissive properties and various applications of UCNPs. Lastly, the challenges and future perspectives of UCNPs are provided as a conclusion.

Nanoparticle-based theranostics combines tumor imaging and cancer therapy in one platform, but the synthesis of theranostic agents is impeded by chemical groups on the surface and the size and morphology of the components. Strategies to construct a multifunctional platform for bioimaging and photothermal therapy (PTT) are urgently needed. A new upconversion-magnetic agent (FeCUPs) based on hollow carbon spheres, which is both a photothermal agent and a dual carrier of luminescent and magnetic nanoparticles, provides an effective approach for tumor elimination.

Nanoscale metal–organic frameworks (MOFs) have attracted widespread interest due to their unique properties including a tunable porous structure, high drug loading capacity, structural diversity, and outstanding biocompatibility. MOFs have been extensively explored as drug nanocarriers in biotherapeutics. However, by harnessing the functionality of ligands and metal ions or clusters in MOFs, the applications of MOFs can be extended beyond drug delivery vehicles. Based on the intrinsic properties of the components of MOFs (e.g. magnetic moments of metal ions and fluorescence of ligands), different imaging modes can be achieved with varied MOFs. With careful design of the composition of MOFs (e.g. modification of organic linkers), they can respond to tumor microenvironments to realize on-demand treatment. By incorporating porphyrin-based ligands (photosensitizers for photodynamic therapy) or high-Z metal ions (radiosensitizers for radiotherapy) into the scaffold of MOFs, MOFs themselves can act as anticancer therapeutic agents. In this review, we highlight the application of MOFs from the above-mentioned aspects and discuss the prospects and challenges for using MOFs in stimuli-responsive imaging-guided antitumor therapy.