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This work presents a portable polarimetric multispectral imaging (PMSI) system operating in the visible to shortwave infrared range (VNIR–SWIR: 400–1700 nm) and its application to target detection, discrimination from aquatic backgrounds, and polymer identification. The instrument integrates two synchronized cameras with motorized bandpass filters and piezoelectric polarization control, enabling the acquisition of 48 wavelength–polarization measurements per capture. This configuration allows the extraction of both intensity-based and polarimetric features, including the degree of linear polarization (DoLP). A complete radiometric and polarimetric calibration framework is implemented, encompassing system response characterization, polarization-dependent gain correction, and reflectance normalization under variable illumination. Experiments conducted on a representative set of 16 polymer materials show that polarimetric information consistently improves class separability compared to intensity-only features, with a mean gain of 6.9 (95% CI: 6.35–8.47). Although the correlation between intensity- and DoLP-based separability is moderate (r = 0.44), the results indicate complementary identification capability. Material recoverability was further evaluated using spectral unmixing techniques (VCA, N-FINDR, and PPI), with VCA offering the best accuracy–complexity trade-off on the calibrated Stokes reflectance dataset. Despite these gains, identification among chemically similar polyethylene variants remains challenging due to limited spectral and polarimetric contrast. An underwater detectability study under natural illumination reveals strong wavelength-dependent constraints: SWIR penetration is limited to 4 cm, whereas VNIR bands (430–550 nm) preserve detectability up to 20 cm, with DoLP enhancing edge visibility. These results motivate future validation in more complex aquatic conditions and with increased spectral dimensionality.