Although the Cambrian marine shale in the Tarim Basin is usually considered to be the source rocks for overlying conventional reservoirs, its unconventional shale-gas potential has not yet been evaluated. To indicate the unconventional resource play potential and highlight more favorable zones, we conducted a comprehensive lithologic, petrophysical, and geochemical analysis of 228 drill core samples from 14 wells and 167 outcrop samples from eight geologic sections in the basin. The results indicate that the Cambrian marine shale was deposited in basinal and slope environments dominated by shale and siliceous shale. The average total organic carbon (TOC) content of the Є1xd (Xidashan) and Є2m (Moheershan) Formations ranges from 0.5% to 2.5%, and that of the Є1y (Yuertusi) Formation ranges from 1.0% to 7.0%. Phytoplankton is dominant in the Є1xd and Є2m Formations, whereas benthic algae are more prevalent in the Є1y Formation. The organic matter ranges in maturity from high to postmature. The shale consists of abundant meso- and macropores. The mineral matter is mostly composed of quartz ( in most samples) followed by carbonate minerals, with minor contributions made by clay minerals (). The analysis of methane adsorption isotherm indicates a positive correlation between the gas and TOC content and a negative correlation between the gas content and burial depth implying the good adsorption capacity of the shale-gas play. Resource estimation of the Middle-Lower Cambrian indicates that the Yuli and Ruoqiang areas contain a potential of shale gas, and they are the most favorable zones for further exploitation.