Surface soil moisture (SSM) estimation is of great importance in several areas, such as hydrology, agriculture and risk assessment. C-band SAR (synthetic aperture radar) data have been widely used to estimate SSM, whereas few studies have been performed using L-band SAR due to the low availability of L-band SAR data. In this context, the objective of the present paper is to compare the SSM estimation potentials of the C- (Sentinel-1) and L-bands (PALSAR) for wheat and grassland plots. The inversion approach developed in this study uses neural networks to invert the SAR signal and estimate the SSM. For each radar frequency, the developed neural networks were trained using the following as an input vector: SAR incidence angle, SAR polarization (VV for the C-band and HH for the L-band), and NDVI from optical images. Artificial Neural networks (ANNs) were developed and validated using synthetic and real databases. The results showed that the L-band provided slightly less accurate SSM estimates than the C-band. Moreover, the results showed that the accuracies of the SSM estimates for both frequencies strongly depended on the soil roughness (Hrms) and SSM values. From the synthetic database at SSM values less than 25 vol.%, the ANNs underestimated the SSM for Hrms values less than 1.5 cm and overestimated the SSM for Hrms values greater than 1.5 cm. In addition, the ANNs underestimated the SSM value regardless of the Hrms value when the SSM value was greater than 25 vol.%. An RMSE analysis of the SSM estimates showed that the highest RMSE values were observed for the L-band regardless of the SSM value, and high RMSE values were observed for the C-band only in very wet soil conditions (SSM>25 vol.%). From the real database at NDVI values less than 0.7, the RMSE (root mean square error) of the SSM estimates was 4.6 vol.% for the C-band and 5.3 vol.% for the L-band. Most importantly, the L-band enabled the estimation of the SSM under a well-developed vegetation cover (NDVI > 0.7) with an RMSE of 6.7 vol.%, whereas the C-band SAR signal became completely attenuated for some crops when the NDVI value was greater than 0.7, and thus the estimation of SSM was impossible using the C-band.