Accurate characterization of dental surface energetics is essential for understanding tooth–restorative adhesion and guiding materials design. Conventional approaches often rely on temperature-independent molecular areas, simplified dispersive interactions, and linear Lewis acid–base models, potentially introducing systematic uncertainties. This study proposes a unified inverse gas chromatography framework integrating the Hamieh models to reassess the surface thermodynamics of enamel, dentin, dental adhesives, resin composites, and glass ionomer cements. The methodology combines thermodynamically consistent adsorption calculations, temperature-dependent molecular surface areas and intermolecular separation distances, corrected London–Hamaker dispersive interactions, and a nonlinear five-parameter Lewis acid–base formulation incorporating amphoteric coupling and second-order interactions. A systematic procedure is established for critically reassessing published dental surface-energy results and identifying potential methodological inconsistencies. Corrected molecular descriptors are subsequently incorporated into a conditional adhesion framework accounting for dispersive and polar interactions, hydration, and surface conditioning. Model applicability is addressed through parameter-identifiability analysis, uncertainty propagation, comparative statistical evaluation, and proposed independent experimental validation. Particular emphasis is placed on distinguishing molecular adsorption thermodynamics from reversible interfacial adhesion and mechanical bonding performance. This framework provides a theoretical and methodological foundation for improving dental surface characterization, evaluating conventional thermodynamic assumptions, and supporting the rational design of restorative materials with enhanced interfacial compatibility.