Plasmonic structural color originates from the scattering and absorption of visible light by metallic nanostructures. Stacks consisting of thin, disordered semicontinuous metal films are attractive plasmonic color media, as they can be mass-produced using industry-proven physical vapor deposition techniques. These films are comprised of random nano-island structures of various sizes and shapes resonating at different wavelengths. When irradiated with short-pulse lasers, the nanostructures are locally restructured, and their optical response is altered in a spectrally selective manner. Therefore, various colors are obtained. We demonstrate the generation of structural plasmonic colors through femtosecond laser modification of a thin aluminum film–isolator–metal mirror (TAFIM) structure. Laser-induced structuring of TAFIM’s top aluminum film significantly alters the sample’s specular and diffuse reflectance depending on the fluence value and the number of times a region is scanned. A “negative image” effect is possible, where a dark field observation mode image is a negative of a bright field mode image. This effect is visible using an optical microscope, the naked eye, and a digital camera. The use of self-passivating aluminum results in a long-lasting, non-fading coloration effect. The reported technique could be used in anti-counterfeiting and security applications, as well as in plasmonic color printing and macroscopic and microscopic marking for personalized fine arts and aesthetic products such as jewelry.