Lanthanum/gadolinium zirconate coatings are deposited via suspension plasma spray with suspensions fabricated by a planetary mill and compared with hot-pressed samples via solid-state reaction. With increase in processing time of the planetary mill, the mean size and BET surface area change rapidly in the case of lanthanum oxide powder. By using suspensions of planetary-milled mixture between lanthanum or gadolinium oxide and nano zirconia, dense thick coatings with fully-developed pyrochlore phases are obtained. The possibilities of these SPS-prepared coatings for TBC application are also discussed.