Roasting can increase the Maillard reaction and caramelization of sweet potatoes to create an attractive appearance, color, aroma, and taste, and is rapidly increasing in the commercial market. This study mainly analyzed the influence of roasting sweet potatoes, with and without the peel, on sweet potato quality and flavor characteristics combined with sensory qualities. The results showed that the a* value (1.65–8.10), browning degree (58.30–108.91), total acidity (0.14–0.21 g/100 g, DW), and maltose content (0.00–46.16 g/100 g, DW) of roasted sweet potatoes increased with roasting time. A total of 46 volatile compounds were detected and 2-furanmethanol, furfural, and maltol were identified as the main sources of the aroma of roasted sweet potatoes. A sensory evaluation based on a comprehensive nine-point acceptance test and descriptive analysis showed that roasting for 1 to 2 h resulted in the highest acceptance score (6.20–6.65), including a golden-yellow color, sweet taste, and fibrous texture. The sweet potatoes became brown after roasting for 2.5 to 3 h and gained a burnt and sour taste, which reduced the acceptance score (4.65–5.75). These results can provide a reference for increased quality in the food industry production of roasted sweet potatoes.