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It is difficult to quantify the amount of chlorophyll fluorescence emitted by a leaf or canopy under natural sunlight because the reflected light obscures the fluorescence signal. In this study, two diurnal experiments were conducted on winter wheat (Triticum aestivum L.) and Japan Creeper (Parthenocissus tricuspidata) to detect the solar-induced chlorophyll fluorescence from field radiance spectra. In the separation of the fluorescence emissive signal from canopy radiance spectrum based on Fraunhofer lines, two Fraunhofer lines of the terrestrial oxygen absorption at 688 and 760 nm were observed in the radiance spectra by an Analytical Spectral Devices FieldSpec Pro NIR spectrometer, which largely overlaps the chlorophyll fluorescence emission spectrum of leaves. Therefore, Fraunhofer lines at 688 and 760 nm were selected to detect the emissive fluorescence. The diurnal changes of chlorophyll fluorescence in the two experiments were primarily affected by the diurnal changes of photosynthetically available radiation (PAR). The correlation coefficients (R2) were greater than 0.9 for all the relationships between PAR and the solar-induced fluorescence of winter wheat and Japan Creeper at 688 and 760 nm based on Fraunhofer line-depth (FLD), suggesting that the solar-induced fluorescence could closely track the changes of PAR and chlorophyll fluorescence. The relative solar-induced fluorescence based on FLD was negatively related to Fv/Fm measured by an OS1-FL modulated chlorophyll fluorometer. The correlation coefficients (R2) were 0.97 at 688 nm and 0.99 at 760 nm for winter wheat, and 0.79 at 688 nm and 0.78 at 760 nm for Japan Creeper. These results demonstrate that the solar-induced fluorescence from plant canopies can be detected from field radiance spectra based on the Fraunhofer line principle.