Simultaneous estimation of thermal properties can be challenging, especially when the parameters are temperature-dependent. Previous research has shown that by using a complementary experiment, temperature-dependent thermal conductivity can be estimated using a single experiment. The objective of this study was to optimize the complementary experiments that can facilitate the simultaneous estimation of temperature-dependent thermal conductivity and volumetric heat capacity. A theoretical study was conducted with two experiments in a single trial with the sample being kept in a cylindrical sample holder, which had a thin film heater in the center. The first part of the experiment was conducted by keeping the external surface temperature at 50 °C for 300 s and allowing the center temperature to equilibrate with the boundary temperature. Then, the second part of the experiment followed, where the thin film heater was supplied with electrical power to increase the center temperate to 140 °C. Several heating profiles were studied to maximize the information obtained from the complementary experiments, and the best one was the power profile with a sinusoidal function. All four parameters of sweet potato puree temperature-dependent thermal conductivity (0.509 to 0.629 W/mK at 25 °C and 140 °C, respectively) and volumetric heat capacity (3.617 × 106 to 4.180 × 106 J/m3K at 25 °C and 140 °C, respectively) were estimated with low standard errors.