A recently proposed protocol enables the acquisition of two-dimensional nuclear magnetic resonance (2D NMR) spectra within a single scan. A promising application opened up by this new data acquisition mode concerns its combination with active nuclear polarization methods, whereby spectroscopy is carried out on analytes whose spin magnetizations have been significantly enhanced over their Boltzmann thermal values. The present paper explores the potential of such combination, with the acquisition of peptide and protein 2D NMR 1H correlation spectra recorded after the samples had been subject to laser-driven chemically induced dynamic nuclear polarization (CIDNP). It is demonstrated that the speed and sensitivity enhancement afforded by these combined processes enables the acquisition of quality 2D NMR data sets within a fraction of a second, at analyte concentrations that are under 1 mM.