Soil moisture is a pivotal hydrological variable that links the terrestrial water, energy, and carbon cycles. In this article, a new soil moisture (SM) index (SMI), which aims to capture the temporal variability of SM, irrespective of cloud cover and solar illumination, was developed by using the L-band SM active passive (SMAP) radiometer observations. The SMI was proposed on the basis of two key foundations: 1) vegetation and roughness have similar effects on “depolarization” of microwave emission, while SM enhances polarization differences and 2) vegetation and roughness generally impose positive effects on surface emissivity, while SM and emissivity are negatively correlated. Based on the two physical principles, it is possible to decouple the effects of SM and those of vegetation and surface roughness in a 2-D space independent of vegetation type and roughness condition. The proposed SMI was then validated by in situ measurements from five dense SM networks covering different vegetation and climatic conditions and also compared with SMAP passive and European space agency climate change initiative (ESA CCI) SM products at a coarse resolution of 36 km, and SMAP-enhanced passive and Japan Aerospace Exploration Agency (JAXA) advanced microwave scanning radiometer (AMSR2) SM products at a medium resolution of 9 km. The results show that the new SMI is able to well reproduce the temporal dynamic of SM with a favorable averaged correlation coefficient value of 0.87 and 0.84 at 36 and 9 km, respectively, higher than that of SMAP passive (0.80), SMAP-enhanced passive (0.77), ESA CCI (0.69), and JAXA AMSR2 (0.53). After removing the systematic differences between satellite and site-specific SM data by using the cumulative distribution function (CDF) matching technique, the SMI can achieve an average root mean squared error (RMSE) of 0.031 and 0.036 m3m−3 at 36 and 9 km during the validation period, respectively, lower than that of the satellite SM products. In addition to surface temperature, the SMI does not need any further information from other sensors [e.g., the optical normalized difference vegetation index (NDVI) or leaf area index (LAI) data] to guarantee an all-weather monitoring. Therefore, it has great potential to estimate SM variability on a global scale.