A triplet-triplet annihilation-based upconversion (TTA-UC) system, employing a multichromophore assembly, is convenient to harvest low-energy photons for light energy conversion and optoelectronic applications. The primary donor in the TTA-UC system, typically a low-bandgap semiconductor, captures the low-energy photons and transfers triplet energy to an annihilator dye molecule, which in turn generates a high-energy singlet excited state via T-T annihilation. We have now succeeded in revealing kinetic and mechanistic details of multistep energy transfer processes in the CsPbI