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Interfacial interaction amongst the antidepressant drug-imipramine hydrochloride (IMP) and pharmaceutical excipient (triton X-100 (TX-100-nonionic surfactant)) mixed system of five various ratios in dissimilar media (H₂O/50 mmol·kg⁻¹ NaCl/250 mmol·kg⁻¹ urea) was investigated through the surface tension method. In addition, in the aqueous solution, the ¹H-NMR, as well as FT-IR studies of the studied pure and mixed system were also explored and deliberated thoroughly. In NaCl media, properties of pure/mixed interfacial surfaces enhanced as compared with the aqueous system, and consequently the synergism/attractive interaction among constituents (IMP and TX-100) grew, whereas in urea (U) media a reverse effect was detected. Surface excess concentration (<i>Γ_max</i>), composition of surfactant at mixed monolayer (<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><msubsup><mi>X</mi><mn>1</mn><mi>σ</mi></msubsup></mrow></semantics></math></inline-formula>), activity coefficient (<i>f</i>₁^σ (TX-100) and <i>f</i>₂^σ (IMP)), etc. were determined and discussed thoroughly. At mixed interfacial surfaces interaction, parameter (<i>β</i>^σ) reveals the attractive/synergism among the components. The Gibbs energy of adsorption (<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><mo>Δ</mo><msubsup><mi>G</mi><mrow><mi>ads</mi></mrow><mi mathvariant="normal">o</mi></msubsup><mo stretchy="false">)</mo></mrow></semantics></math></inline-formula> value attained was negative throughout all employed media viewing the spontaneity of the adsorption process. The ¹H NMR spectroscopy was also employed to examine the molecular interaction of IMP and TX-100 in an aqueous system. FT-IR method as well illustrated the interaction amongst the component. The findings of the current study proposed that TX-100 surfactant could act as an efficient drug delivery vehicle for an antidepressant drug. Gels can be used as drug dosage forms due to recent improvements in the design of surfactant systems. Release mechanism of drugs from surfactant/polymer gels is dependent upon the microstructures of the gels and the state of the drugs within the system.