A spectrally tunable light source utilizing three light-emitting diodes (LEDs) for calibration of a highly sensitive intensified charge-coupled device (ICCD) optical detection system intended for time-resolved galvanoluminescence (GL) measurements is described. The source has been conceived as a low-cost substitute for standard tungsten lamps usually used for relative and absolute calibration of optical detection systems. Three LEDs with different spectral characteristics in conjunction with a system of two integrating spheres as light mixers and light reducers are used. This construction provides control over the source spectrum by changing individual LED contributions. The use of integration spheres eliminated angular distribution of light intensities of LEDs as well as angular dependence of their spectral contributions. Moreover, by using the source we have avoided the problem of stray and diffuse light of higher wavelengths, as well as different light intensities for different wavelengths (up to three orders of magnitude in the range from 400 nm to 750 nm), which we have with standard tungsten lamps. A complete calibration procedure for the LED source and ICCD detection system is described. Finally, for the first time, we have performed time-resolved spectral GL measurements during aluminum anodization in porous film-forming electrolyte phosphoric acid in a transient regime. Two peaks at 425 nm and 595 nm are recognized, confirming the same mechanism of GL in both transient and steady-state regimes of anodization.