NMR detection in the ultralow-field regime (below 10 μT) was used to measure the nuclear spin relaxation rates of liquids imbibed into silica pellets with mean pore diameters in the 10-50 nm range. Heptane, formic acid and acetic acid were studied and relaxation rate data were compared with a conventional field-cycling NMR technique. Detection of 1H-13C spin coupling NMR signals at zero field (∼0.1 nT) allowed spectroscopic identification of molecules inside the porous material and unambiguous measurements of the chemistry-specific relaxation rates in liquid mixtures. In the case of molecules that contain 1H and 13C, spin-singlet state relaxation can provide additional information about the dynamics. Applications and future improvements to the methodology are discussed.