LAUSR

Abstract Upconverting materials have achieved great progress in recent years, however, it remains challenging for the mechanistic research on new upconversion strategy of lanthanides. Here, a novel and efficient strategy to realize photon upconversion from more lanthanides and fine control of lanthanide donor–acceptor interactions through using the interfacial energy transfer (IET) is reported. Unlike conventional energy‐transfer upconversion and recently reported energy‐migration upconversion, the IET approach is capable of enabling upconversions from Er3+, Tm3+, Ho3+, Tb3+, Eu3+, Dy3+ to Sm3+ in NaYF4‐ and NaYbF4‐based core–shell nanostructures simultaneously. Applying the IET in a Nd–Yb coupled sensitizing system can also enable the 808/980 nm dual‐wavelength excited upconversion from a single particle. More importantly, the construction of IET concept allows for a fine control and manipulation of lanthanide donor–acceptor interactions and dynamics at the nanometer‐length scale by establishing a physical model upon an interlayer‐mediated nanostructure. These findings open a door for the fundamental understanding of the luminescence dynamics involving lanthanides at nanoscale, which would further help conceive new scientific concepts and control photon upconversion at a single lanthanide ion level.