The necessity of augmentation for oil shale explorations has led to increasing theoretical and technical requirements regarding online and direct detection of the organic content in shale. In this study, an ultraviolet laser with a wavelength of 248 nm is employed to analyze the oil shales with different oil yields and from different oil fields. Experimental results found that the laser-induced voltage (LIV) was monotonically related to the organic contents in the shale. Also, the LIV peaks linearly increased with an increase in the laser intensity and oil yield. Organics, like kerogen, and inorganic minerals reflected different energy bands. The higher the oil yield of the shale, the more the carriers were excited by the laser, indicating a stronger built-in electric potential. The microscopic structures, minerals, and kerogen were determined using a scanning electron microscope, X-ray diffraction, and Raman spectroscopy. The results showed that LIV can directly detect the organic content of oil shale for use in geophysical prospecting in the unconventional oil-gas resources industry.