Tetracycline (TC) is one of the most frequently detected antibiotics in various water matrices, posing adverse effects on aquatic ecosystems. In this study, coconut shell-based powdered activated carbon (PAC) was thermally modified under various temperatures to enhance TC adsorption. The PAC subjected to 800 °C (PAC800) showed the best TC adsorption. PAC and PAC800 were characterized using N2 adsorption/desorption isotherm, X-ray photoelectron spectroscopy, Raman spectroscopy, XRD, Boehm titration, and zeta potential analyses. Increases in the specific surface area, C/O ratio, C=O, surface charge, basic groups, and the number of stacked graphene layers along with a decrease in structural defects were observed for PAC800 compared to PAC. The TC adsorption was significantly improved for PAC800 compared to that of PAC, which is attributable to the enhanced electrostatic attraction and π-π EDA interactions induced by the changes in the properties. The Freundlich isotherm was the best fit indicating the heterogeneous nature, and the Freundlich constant of PAC and PAC800 increased from 85.8 to 119.5 and 132.1 to 178.6 (mg/g)‧(L/mg)1/n, respectively, when the temperature was increased from 296.15 to 318.15 K. The kinetics were well described by the pseudo-second-order adsorption model and the rate constant of PAC and PAC800 increased from 0.80 to 1.59 and from 0.72 to 1.29 × 10−3 g/mg‧min, respectively, as the temperature was increased. The activation energy of PAC and PAC800 was 23.7 and 19.6 J/mol, respectively, while the adsorption enthalpy was 196.7 and 98.5 kJ/mol, respectively, indicating endothermic nature. However, it was suggested that TC adsorption onto PAC800 was more favorable and was more contributed to by physisorption than that onto PAC. These results strongly suggest that the properties, adsorption capacity, and adsorption mechanisms of carbonaceous adsorbents can be significantly changed by simple thermal treatment. More, the results provide valuable information about the design of carbonaceous adsorbents with better performance where the structures and functional groups, which positively affect the adsorption, must be improved.