The relationship between the photometric, electric, and thermal parameters of light-emitting diodes (LEDs) is important for optimizing the LED illumination design. Indium gallium aluminium phosphide (InGaAlP)-based thin-film surface-mounted device (SMD) LEDs have attracted wide attention in research and development due to their portability and miniaturization. We report the optical characterization of InGaAlP thin-film SMD LED mounted on FR4, 2 W, and 5 W aluminum (Al) packages. The optical and thermal parameters of LED are determined at different injection currents and ambient temperatures by combining the T3ster (thermal transient tester) and TeraLED (thermal and radiometric characterization of power LEDs) systems. Analysis shows that LED on a 5 W Al substrate package obtains the highest luminous and optical efficiency.