This data set contains all the data presented in the main text figures and extended data figures (for the manuscript titled 'Operando optical tracking of single-particle ion dynamics in batteries'). The information on how the data was acquired and processed is detailed in the open access manuscript + SI which has been deposited in this repository. Main Figures: Figure1: (Panel b) Galvanostatic cycling data of LCO (voltage vs specific capacity) for 5 cycles at 2C. (Panel c) Corresponding differential capacity data (dQ/dV vs voltage). (Panel f) Raw iSCAT image and SEM image of a LCO particle. Figure 2: (Panel a) Voltage, differential capacity, and mean iSCAT intensity from an individual LCO particle, during a galvanostatic cycle (Cycle4) at 2C. (Panel b) Background subtracted iSCAT images of an individual LCO particle throughout cycling. Figure 3: (Panel a&b) Sequential differential images showing phase boundary movement during the biphasic transition, in delithiation and lithiation. (Panel c&d) The fraction of the new phase within the particle over time, and the corresponding single particle biphasic C-rates. Figure 4: (Panel a) Voltage vs cell capacity curves and corresponding single-particle intensity behaviour, over a range of C-rates from C/2 to 6C. (Panel b&c) Single particle biphasic C-rates during these cycles at a range of applied C-rates, for both delithiation and lithiation. (Panel d) Time maps showing the progression of phase boundaries through a single particle, during the biphasic transitions, at a range of C-rates. Figure 5: (Panel a&b) Total differential images showing intensity changes in a single particle caused by the lithium ordering transition. Delithiation and lithiation images are each included for two separate cycles. (Panel e&f) Sequential differential images during the disordering upon lithiation, showing the progression of the disordered phase through the particle, for two separate cycles. Extended Data Figures: Extended data figure 1: (Panel b) XRD patterns of both the pristine LCO powder, and the LCO electrode. (Panel c) List of measured particle diameters (used in the figure to construct a histogram of particle sizes). (Panel d-i) SEM and raw iSCAT images of LCO particles within the electrode. Extended data figure 2: (Panel a) Galvanostatic cycling data of LCO (voltage vs specific capacity) for 5 cycles at 2C, in a coin cell and in an optical cell. (Panel d) Corresponding differential capacity data (dQ/dV vs voltage). Extended data figure 3: Voltage and mean iSCAT intensity from an individual LCO particle, during 5 galvanostatic cycles at 2C. Extended data figure 5: Sequential differential images showing phase boundary movement through a single particle, during the biphasic transition, in delithiation and lithiation, for 5 cycles. Extended data figure 6: Total differential images showing intensity changes in a single particle caused by the lithium ordering transition. Delithiation and lithiation images are each included for 5 separate cycles.