Developing light-harvesting materials with tunable emission colours has always been at the forefront of colour display technologies. The variation in materials composition, phase and structure can provide a useful tool for producing a wide range of emission colours, but controlling the colour gamut in a material with a fixed composition remains a daunting challenge. Here, we demonstrate a convenient, versatile approach to dynamically fine-tuning emission in the full colour range from a new class of core-shell upconversion nanocrystals by adjusting the pulse width of infrared laser beams. Our mechanistic investigations suggest that the unprecedented colour tunability from these nanocrystals is governed by a non-steady-state upconversion process. These findings provide keen insights into controlling energy transfer in out-of-equilibrium optical processes, while offering the possibility for the construction of true three-dimensional, full-colour display systems with high spatial resolution and locally addressable colour gamut.