The thermodynamics of mixed micellization of amitriptyline hydrochloride (AMT) with ionic liquid-type imidazolium gemini surfactant ([C 10 -4-C 10 im] Br 2 ), was investigated at different mole fractions and temperatures by surface tension measurements. The deviation of the critical micelle concentration (CMC) from the ideal critical micelle concentration (CMC*), micellar mole fraction (X m 1 ) from ideal micellar mole fraction (X ideal 1 ), the values of interaction parameter (b) and activity coefficients (f i ) (for both mixed micelles and mixed monolayer) explained the non-ideal behavior (i.e., synergistic behavior) of binary mixtures. The excess free energy (DG ex ) for the AMT-[C 10 -4-C 10 im] Br 2 binary mixtures explained the mixed micelles stability in comparison to micelles of [C 10 -4-C 10 im] Br 2 and pure AMT. Interfacial parameters, i.e., Gibbs surface excess (C max ), minimum head group area at air/water interface (A min ), free energy of micellization (DG o m ), and standard Gibbs energy of adsorption (DG ads o ) were also evaluated for the systems. The standard entropy of adsorption (DS ads o ) was found higher than the standard entropy of micellization (DS m o ) at all mole fractions of AMT (a 1 ).