To expand and investigate the potential of spectral imaging, we developed a portable multispectral system using light-emitting diodes. This system recovers spectral information from the UV to the near IR over a large area using two different image sensors synchronized with 23 bands of illumination. The system was assessed for spectral reconstruction through simulations and experimental measurements by means of two methods of spectral reconstruction and three different evaluation metrics. The results over a Macbeth ColorChecker chart and other samples, including pigments usually employed in art paintings, are compared and discussed. The portable multispectral system using LEDs constitutes a cost-effective and versatile method for spectral imaging.