This work presents experimental data on the density (ρ), viscosity (η), and surface tension (γ) of monoethanolamine (MEA), diethylenetriamine (DETA), and their binary mixed solutions across 298.15–318.15 K. Using these physicochemical data, the work also explored properties like excess molar volume (VmE) and viscosity deviation (Δη) of the solutions. The experimental results were modeled using the Jouyban-Acree model, McAllister four-body model, and Redlich-Kister (R-K) equation. The application of these parametric models confirmed strong intermolecular interactions (The length (1.911 Å) and energy (HF value: −2237.54 kJ/mol and Des: −21.61 kJ/mol) of hydrogen bond) within the MEA + DETA binary mixed solutions. Spectroscopic analyses, including Raman and nuclear magnetic resonance hydrogen spectroscopy, revealed the presence of intermolecular hydrogen bonding (OH⋯N(H2)) in the MEA + DETA binary mixed solutions. Lastly, the CO2 absorption capacity of the solutions was experimentally studied, providing a theoretical foundation and reference data for future experiments and process design of CO2 capture.