Lanthanide luminescence is presented in full spectral and temporal detail by challenging the limits of low-light sensing and high-speed data acquisition. A robust system is demonstrated, capable of constructing high-resolution time-resolved spectra with high throughput processing. This work holds real value in advancing characterisation capability to decode interesting insights within lanthanide materials.By meeting the stringent requirements in lighting, telecommunication, electroluminescent devices, analytical sensors and bioimaging set-ups, the luminescence properties of lanthanide-doped materials have attracted significant research efforts both at the fundamental and applied levels.1 The unique luminescent properties of lanthanide materials offer sharp emission spectrum, large Stokes shifts, exceptionally long lifetime, and upconversion generation that stem from their ladder-like energy levels and sophisticated energy transfer processes. Traditional spectroscopic approaches of either luminescence spectra or lifetime decay rates at individual wavelengths are insufficient to understand the rich chemical physics. This deficiency as result of lacking of robust instrumentation development remains a major barrier for the field of material science and applications. 16 In the NaYF 4 :Yb/Er system, a network of closely spaced Yb ions sensitises with infrared radiation at a wavelength of 980 nm and couples via non-radiative resonance to neighbouring Er ions. In contrast with organic dye fluorophores, the Er ion has multiple excited states with remarkably long (subms) lifetimes, so that upconversion nanocrystals are able to stepwise absorb two or more near-infrared photons, and display blueshifted emission in the visible spectrum. Fundamental to fully understand the mechanisms behind upconversion process in Ln-doped nanocrystals, one must overcome the difficulties that result from multiple energy levels of the lanthanide material itself and the complicated photon relaxation process associated with multiple sensitised photons travelling within a network of thousands of interacting nano-scaled sensitisers and emitters, which together are influenced by the large surface-to-volume ratio common in nanoparticle science. 17 Practically, there are two major properties of the upconversion luminescence that provide opportunities for advanced bioimaging. 12 Firstly, in the spectral domain, narrow-bandwidth anti-Stokes-shifted emission allows efficient colour separation from the autofluorescence. The second advantage lies in a millionfold difference between the much longer lifetimes of upconversion nanocrystals and shorter endogenous fluorophores lifetimes that make up the autofluorescence background (y1 ms cf. y3 ns). Therefore an optical time-gated approach allows almost complete suppression of the autofluorescence and excitation background. From an application perspective, it becomes critical to characterise simultaneously the spectral and lifetime characteristics of Lndoped nanocrystals as a unifying picture. There have been ...