The light emitting diode (LED) development technology is an important topic for green industry. This study focused on the efficient cleaning for LAO hydrolysis material, which is a potential LED substrate. The 99.5% ethanol or an alternative solution is used to clean the LAO substrate and dry with the help of anhydrous gas. To improve the cleaning performance, the Taguchi-based orthogonal array of experimental planning and the Grey Relation Analysis are employed to optimize the cleaning parameters. Four control factors are cleaning time, soaking time, PVA sponge type, drying method. The multiple performance characteristics of responses include the residual traces of impurities and water mark after the cleaning process for LAO substrate. With the proposed cleaning process, the surface foreign matter removal rate of target 80% and the residual water marks of declining to 20% are achieved.