In this work, three different TBC compositions comprising of yttria partially stabilized zirconia (8YSZ), yttria fully stabilized zirconia (48YSZ) and gadolinium zirconate (GZ) respectively, were processed by suspension plasma spray (SPS) to obtain columnar microstructured TBCs. Additionally, for comparison, lamellar microstructured, 7YSZ TBC was deposited by air plasma spray (APS) process. SEM analysis was carried out to investigate the microstructure and white light interferometry was used to evaluate the surface morphology of the as-sprayed TBCs. Porosity measurements were made using water intrusion and image analysis methods and it was observed that the SPS-YSZ and APS-YSZ TBCs showed higher porosity content than SPS-GZ and SPS-48YSZ. The as-sprayed TBC variations (APS-YSZ, SPS-YSZ, SPS-GZ, and SPS-48YSZ) were subjected to erosion test. Results indicate that the erosion resistance of APS-YSZ TBC was inferior to the SPS-YSZ, SPS-GZ and SPS-48YSZ TBCs respectively. Among the SPS processed TBCs, SPS-YSZ showed the highest erosion resistance whereas the SPS-48YSZ showed the lowest erosion resistance. SEM analysis of the eroded TBCs (cross section and surface morphology) was performed to gain further insights on their erosion behavior. Based on the erosion results and post erosion SEM analysis, erosion mechanisms for splat like microstructured APS TBC and columnar microstructured SPS TBCs were proposed. The findings from this work provide new insights on the erosion mechanisms of columnar microstructured TBCs and lamellar microstructured TBCs deposited by plasma spray.