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The polarimetric Synthetic Aperture Radar (SAR) data sets have been widely exploited for land use land cover (LULC) classification due to their sensitivity to the structural and dielectric properties of the imaging target. In this study, the potential of fully polarimetric L‐ and S‐band Airborne SAR (LS‐ASAR) data sets were explored for the machine‐learning‐based classification of Urban, Vegetation, Waterbody, and Open Ground. This work was done by utilizing dual‐frequency L‐ and S‐band airborne data of Santa Barbara, California, USA, acquired under the Airborne SAR (LS ASAR) campaign, a precursor airborne mission to the space‐borne NASA‐ISRO (NISAR) mission. The LS‐ASAR polarimetric information was utilized for LULC classification using the SVM classifier. The roll‐invariant Barnes, and eigenvalue/eigenvector‐based Cloude and H/A/Alpha decomposition were implemented to retrieve the scattering parameters. The backscatter response of classes was studied, and separability analysis was done to reduce the misclassification error between six class pairs‐ Vegetation—Urban, Vegetation—Waterbody, Vegetation—Open Ground, Urban—Waterbody, Urban—Open Ground, and Water—Open Ground. The decomposition models failed to achieve the desirable separability index for all six class pairs; consequently, the classification of Barnes, Cloude, H/A/Alpha decomposition showed misclassification between vegetation‐urban class, and waterbody‐open ground class for both L‐ and S‐band data sets. The effort was made toward improving the classification accuracy by integrating the roll‐invariant and eigenvalue‐eigenvector scattering parameters of the multifrequency L‐ and S‐band data set. This method presented the desirable separability index for all class‐pair; eventually highest classification accuracy was achieved i.e. 93.35% (kc ${k}_{c}$ = 0.91) by significantly reducing the misclassification error between class pairs. Key Points: Implementation of Barnes, Cloude & H/A/Alpha polarimetric decomposition models on dual‐frequency polarimetry SAR L‐ and S‐band data setsSupport Vector Machine classification of scattering parameters and generation of confusion matrices for Accuracy AssessmentImproving the classification accuracy by integrating the polarimetric scattering components of L‐ and S‐band data sets [ABSTRACT FROM AUTHOR]