The difficulty of accurate and large-scale measurement for surface parameters limits the regional surface soil moisture (SSM) estimation using synthetic aperture radar (SAR). Moreover, the coarse resolution of soil moisture products generated by existing methods, which fuse SAR and passive microwave products, cannot fully satisfy the requirement of specific regional applications. To solve this problem, an SAR-optical data fusion method for soil moisture estimation (SOFSME) based on a cascade neural network is proposed in this study. SOFSME obtains surface parameters from historical soil moisture images and related environmental images to estimate a SSM image with high resolution at large scale from Sentinel-1A C-band SAR data. Validation experiments in single and multiple land-use type areas showed that the SOFSME performed best on bare soil areas with a median root mean square error of 0.0203. The median universal image quality index of estimated soil moisture image was 0.1454, which was better for single cropland areas than multi-land-use type areas. The Pearson correlation coefficient showed a median value of 0.7645 in both experiments. These results showed that the SOFSME had high accuracy, availability, and stability in regional soil moisture estimation. Compared with existing methods, the SOFSME can provide high-quality soil moisture images and does not directly depend on field measurement data. Thus, the proposed SOFSME method is of great value for high-resolution soil moisture estimation in more regional applications.