An enhanced sensitivity zero-quantum correlation experiment is proposed for recording H-1-C-13 correlations of methyl groups in highly deuterated, methyl protonated large proteins. The zero-quantum spectra benefit from TROSY-effects in which both intra- and inter-methyl dipolar relaxation interactions are minimized. Applications to malate synthase G at 5degreesC (81 kDa single polypeptide chain enzyme, correlation time of 118 ns) and lysine decarboxylase at 45degreesC (810 kDa decameric enzyme) are presented showing significant improvements in resolution relative to corresponding HMQC data sets, with only slight decreases (similar to10%) in sensitivity.