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To mitigate factors that have limited studies of large, functionally relevant RNAs by solution nuclear magnetic resonance (NMR) spectroscopy, we have extended a recently described <jats:sup>2<\/jats:sup>H\u2010enhanced, <jats:sup>1<\/jats:sup>H\u2010<jats:sup>15<\/jats:sup>N correlation approach\u00a0that used uniformly 15N\u2010labeled guanosine triphosphate (GTP) by developing a chemoenzymatic labeling technology that grafts selectively labeled [9\u2010<jats:sup>15<\/jats:sup>N]\u2010Guanine on to any labeled ribose to make [9\u2010<jats:sup>15<\/jats:sup>N]\u2010GTP. The approach exploits advantageous NMR properties of the N9 nucleus which, when combined with extensive ribose deuteration and optimized NMR pulse sequences, affords sharp signals without complications that can arise using uniform [<jats:sup>15<\/jats:sup>N]\u2010guanine labeling. The utility of the approach for NMR signal assignment and dynamics analysis is demonstrated for three large RNAs (20\u201378\u2009kDa) that play critical roles in viral replication. 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