All solid-state lighting products produce heat which should be removed by use of a heat sink. Since the two mating surfaces of light emitting diode (LED) package and heat sink are not flat, a thermal interface material (TIM) must be applied between them to fill the gaps resulting from their surface roughness and lack of coplanarity. The application of a traditional TIM may squeeze out when pressure is applied to join the surfaces and hence a short circuit may result. To avoid such a problem, a thin solid film based TIM has been suggested. In this study, a zinc oxide (ZnO) thin film was coated on Cu substrates and used as the TIM. The ZnO thin film coated substrates were used as heat sink purposes in this study. The prepared heat sink was tested with 3 W green LED and the observed results were compared with the results of same LED measured at bare and commercial thermal paste coated Cu substrates boundary conditions. The influence of interface material thickness on total thermal resistance (Rth-tot), rise in junction temperature (TJ), and optical properties of LED was analyzed. A noticeable reduction in Rth-tot (5.92 K/W) as well as TJ (ΔTJ = 11.83 °C) was observed for 800 nm ZnO thin film coated Cu substrates boundary conditions when compared with bare and thermal paste coated Cu substrates tested at 700 mA. Change in TJ influenced the thermal resistance of ZnO interface material. Improved lux level and decreased correlated color temperature (CCT) were also observed with ZnO coated Cu substrates.