Metallic nanorods exhibit fascinating optical properties due to surface plasmons—collective oscillation of the electron cloud within a particle. They exhibit two principle absorption bands that correspond to surface plasmon resonance (SPR) along the longitudinal and transverse directions of the nanorod. Most importantly, the longitudinal band can be tuned with the aspect ratio of the rod, making it a spectrally tuneable optical material, which can be applied to a variety of devices from bioimaging to high‐density optical storage. Here, spectral encoding for high‐density optical storage applications is demonstrated on two sizes of gold nanorods (aspect ratios of three and five) doped in a silica sol–gel matrix by femtosecond pulsed laser irradiation. It is widely known that high‐power pulsed laser irradiation causes metal nanorods to undergo shape transformations via the process of melting or fragmentation. The process is enhanced if the laser wavelength is tuned at the longitudinal surface plasmon resonance peak of the nanorods, which results in a significant reduction or shift in the surface plasmon resonance peak. As such a shape change occurs only on the subpopulation of rods that have a longitudinal plasmon band matching the laser wavelength, a size‐ or spectrum‐selective shape transition is possible in a rod mixture with varying aspect ratios. The current spectral encoding technology can be incorporated into existing optical disc technology, such as three‐dimensional bit‐by‐bit and holographic, and can increase the capacity limit by utilizing the spectral domain.