Methods for providing improved resistance to CMAS infiltration for hot section components of a gas turbine engine. Exemplary methods include coating a substrate with a thermal barrier coating system by overlying a bond coated substrate with an inner thermal barrier layer comprised of a thermal barrier material such as yttria-stabilized zirconia. A top layer, including a rare-earth aluminate, is deposited so as to overlie at least a portion of the inner layer. Deposition processes and coating thicknesses may be tailored to the type of component to be coated.