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Carbon nanotubes (CNTs) were used to enhance the laser patterning performance of polypropylene (PP). The three-dimensional network structure formed by CNTs can effectively improve the photothermal conversion effect of PP/CNT composites. The results show that the addition of 10 ppm CNTs endowed PP with a clear black laser patterning performance. As the content of CNTs is increased from 10 ppm to 200 ppm, the grayscale of the laser-induced patterns changed from black to white. An amorphous carbon material constituted the laser-induced pattern, which was confirmed by Raman spectroscopy. In addition, the SEM results revealed that the morphology of the laser-induced carbonized points can affect the grayscale of the laser-induced patterns. This study proposes a simple and efficient method for improving the laser patterning performance of polymer materials using CNTs. In addition, this work provides an effective direction for practical applications of grayscale-controlled (black and white) laser-induced patterns.