In this paper, the thermodynamic activity of two lanthanide chlorides (CeCl3 and NdCl3) in molten LiCl-KCl eutectic salt measured using open circuit potentiometry has been reported. Activity coefficient of CeCl3 was found to be strongly dependent on the concentration of CeCl3 in a concentration window of up to 4.66 mol % CeCl3. The activity coefficient of NdCl3 could not be measured due to the uncertainty in NdCl3/NdCl2 molar ratio in the salt, however the thermodynamic activity was measured relative to a 5 mol% Ag∣AgCl reference electrode. The concurrent analysis of data presented in this paper along with previously published activity data for LaCl3 and GdCl3 demonstrates that the departure from ideal solution behavior shown by the rare earths chlorides correlates with ionic size of underlying rare earth element. The smaller the ionic size of the species under consideration, the greater its departure from ideal solution behavior. Further, using the activity data of all four rare earth chlorides, an ionic size dependent correlation was developed. Using this empirical correlation, it is possible to calculate the activity of all species from La(Z = 57) to Gd (Z = 64) for a concentration of up to 2.5 mol% rare earth chloride in LiCl-KCl molten salt at 773 K.