The Soil Moisture and Ocean Salinity (SMOS) satellite mission, based on an aperture synthesis L-band radiometer was successfully launched in November 2009. In the context of a validation campaign for the SMOS mission, intensive airborne and in situ observations were performed in southwestern France for the SMOS CAL/VAL, from April to May 2009 and from April to July 2010. The CAROLS (Cooperative Airborne Radiometer for Ocean and Land Studies) bi-angular (34°-0°) and dual-polarized (V and H) L-band radiometer was designed, built and installed on board the French ATR-42 research aircraft. During springs of 2009 and 2010, soil moisture observations from the SMOSMANIA (Soil Moisture Observing System - Meteorological Automatic Network Integrated Application) network of Météo-France were complemented by airborne observations of the CAROLS L-band radiometer, following an Atlantic-Mediterranean transect in southwestern France. Additionally to the 12 stations of the SMOSMANIA soil moisture network, in situ measurements were collected in three specific sites within an area representative of a SMOS pixel. Microwave radiometer observations, acquired over southwestern France by the CAROLS instrument were analyzed in order to assess their sensitivity to surface soil moisture (w_g). A combination of microwave brightness temperature (T_b) at either two polarizations or two contrasting incidence angles was used to retrieve w_g through regressed empirical logarithmic equations with good results, depending on the chosen configuration. The regressions derived from the CAROLS measurements were applied to the SMOS T_b and their retrieval performance was evaluated. The retrievals of w_g showed significant correlation (p-value < 0.05) with surface measurements for most of the SMOSMANIA stations (8 of 12 stations) and with additional field measurements at two specific sites, also. Root mean square errors varied from 0.03 to 0.09 m³m^-3 (0.06 m³m^-3 on average).