Taikor (Garcinia pedunculata Roxb.) is an underutilized, however nutritious fruit, typically found in Bangladesh and northeast parts of India. Taikor slices (1 ± 0.25 cm thickness) were pretreated for 10 min in 10% sucrose, 10% fructose, and 2% brine solution. Three different temperatures, such as 45, 50, and 55 °C were used to perform the drying operation at 30% constant relative humidity (RH). The thin-layer dehydration characteristics of taikor slices were analyzed using the Newtonian, Page, and Henderson and Pabi’s model. The changes in pH, total acidity, color, β-carotene, vitamin C, B vitamins, antioxidant activity, and microbial load calculation were done to compare the comprehensive quality of untreated and pre-treated dried taikor. After assessing the coefficient of determination (R2) and root mean square error (RMSE) values, the Page model was obtained as the best-suited model. For this model, the R2 and RMSE values were found to be approximately 1 and below 0.1094, respectively. Among the pretreatments, sucrose helped retain quality characteristics like ascorbic acid (115.25 ± 0.19 mg/100 g), antioxidant activity (33.25 ± 0.07%) more in the dried samples. The brine pretreated sample had minimum microbial growth. Fructose pretreated taikor samples dried at 45 °C exhibited maximum value of B vitamins (B1 0.025 ± 0.002 mg/100 g, B2 0.016 ± 0.002 mg/100 g, B3 0.011 ± 0.001 mg/100 g), total phenolic content (15.78 ± 0.15 mg GAE/100 g), total flavonoid content (11.11 ± 0.08 mg QE/100 g). Overall, fructose pretreated sample dried at 55 °C was found to be the best method for preserving the maximum physical and chemical quality of dried Garcinia pedunculata.