High heat transfer performance of spray cooling on structured surface might be an additional measure to increase the safety of an installation against any threat caused by rapid increase in the temperature. The purpose of present experimental study is to explore heat transfer performance of structured surface under different spray conditions and surface temperatures. Two cylindrical stainless steel samples were used, one with pyramid pins structured surface and other with smooth surface. Surface heat flux of 3.60, 3.46, 3.93 and 4.91 MW/m2 are estimated for sample initial average temperature of 600, 700, 800 and 900 °C, respectively for an inlet pressure of 1.0 MPa. A maximum cooling rate of 507 °C/s was estimated for an inlet pressure of 0.7 MPa at 900 °C for structured surface while for smooth surface maximum cooling rate of 356 °C/s was attained at 1.0 MPa for 700 °C. Structured surface performed better to exchange heat during spray cooling at initial sample temperature of 900 °C with a relative increase in surface heat flux by factor of 1.9, 1.56, 1.66 and 1.74 relative to smooth surface, for inlet pressure of 0.4, 0.7, 1.0 and 1.3 MPa, respectively. For smooth surface, a decreasing trend in estimated heat flux is observed, when initial sample temperature was increased from 600 to 900 °C. Temperature-based function specification method was utilized to estimate surface heat flux and surface temperature. Limited published work is available about the application of structured surface spray cooling techniques for safety of stainless steel structures at very high temperature scenario such as nuclear safety vessel and liquid natural gas storage tanks.