Roasting is a critical process that affects the quality attributes of coffee beans; however, how roasting conditions affect the physical, chemical, biological, and organoleptic changes of coffee pulp needs more research. In the present study, we investigated the effects of roasting temperatures and times on chemical compositions and quality attributes of coffee pulp. The results showed that the contents of total soluble sugar (TSS) and free amino acid (FAA) followed a temporal pattern of first increasing and then decreasing under the roasting temperatures between 100 and 160 • C. Total phenolic content (TPC) and antioxidant activity of coffee pulp significantly (p < 0.05) increased after roasting, reaching the maximum values of 83.09 mg gallic acid equivalent (GAE) /g and 360.45 µM 6-hydroxy-2,5,7,8-tetramethylchroman-2-carboxylic acid (Trolox) /g, respectively, when coffee pulp was roasted at 160 • C for 18 min. Drying rates of coffee pulp fitted the Logarithmic kinetic model, while color (L*, a*, and b*) changes and 5-caffeoylquinic acid degradation followed the first-order kinetic model. Electronic nose analysis showed that the main aroma compounds of the coffee pulp are sulfur-containing organics that were reduced with the extended roasting time. Scanning electronic microscopy analysis presented the loosened, shrunk, and cracked microstructure on the surface of the roasted coffee pulp, which might contribute to the increased TSS, FAA, TPC, and antioxidant activity of coffee pulp roasted under specific conditions. In conclusion, our research provides valuable information for preparing high-quality coffee pulp tea.