Texture is a sensory attribute of uppermost importance for the preference of potatoes. In an earlier study, it was shown that sensory texture attributes of boiled potatoes could be predicted, to some extent, by partial least squares regression of relaxation curves obtained from raw potato samples using pulsed low-field1H NMR. The aim of the present study was to understand the chemical background for the low-field NMR prediction of the sensory texture attributes of potatoes. Correlations between low-field NMR relaxation curves, sensory texture attributes and chemical constituents are presented. It is found that prediction of sensory texture quality of boiled potatoes from relaxation curves of raw potatoes is possible mainly because the NMR relaxation curves contain information on water content, which is inversely correlated to starch content. However, low-field NMR seems to offer additional information, which is not included in the chemical variables like starch content. Apparently, adhesiveness and springiness are slightly better described by low-field NMR than by chemical descriptors. This indicates that low-field NMR is able to probe certain mouth-feel variables due to its sensitivity to the state of moisture in the sample, a parameter it is not possible to measure by any other instrumental technique.