AbstractMobile nuclear magnetic resonance (NMR) is a flexible technique for nondestructive characterization of water in plants, the physical properties of polymers, moisture in porous walls, or the binder in paintings by relaxation measurements. NMR relaxation data report material properties and therefore can also help to characterize the state of tangible cultural heritage. In this work, we discuss the relaxation behavior in two series of naturally aged paint mock‐up samples. First, paints with different pigment concentrations were prepared and investigated in terms of the longitudinal and transverse relaxation‐time distributions. We document the evolution of both relaxation‐time distributions during the initial drying stage and demonstrate the heightened importance of transverse over longitudinal relaxation measurements. Second, we observe nonlinear dependences of the relaxation times on the pigment concentration in a typical oil binder. Third, in a study of naturally aged paint samples prepared in the years between 1914 and 1951 and subsequently aged under controlled conditions, we explore the possibility of determining the age of paintings using partial least square regression (PLS) by fitting T1–T2 data with the sample age. Our results suggest some correlation, albeit with significant scatter. Estimating the age of a painting stored under unknown conditions from NMR relaxation data is therefore not feasible, as the cumulative effects of light irradiation, humidity, and biological degradation further obfuscate the chemical and physical impact of aging on the relaxation times in addition to the impact of pigment concentration.