Gari, a fermented granular cassava food product, continues to play a major role in the diets of West Africans. The white cassava commonly used for this product is devoid of provitamin A but may have a significant concentration of cyanogenic compounds. The physicochemical and functional properties of partial substitution of cassava with orange-fleshed sweetpotato (OFSP) to process gari were investigated. Two commonly consumed products “eba” and “soaked gari” were prepared from the various formulations and sensorially assessed. Cassava OFSP composite gari (77% cassava:23% OFSP, 75% cassava:25% OFSP, and 73% cassava:27% OFSP) did not significantly (p > 0.05) influence the moisture content (3.39%−5.42%, p = 0.38), water absorption capacity (589–671 mL/g, p = 0.22), and swelling index (3.75–4.17, p = 0.08) compared with that of 100% cassava gari. Expectedly, increasing the levels of OFSP incorporation significantly (p < 0.001) resulted in color change from white (L* = 83.99, a* = 0.93, b* = 16.35) to orange (L* = 69.26, a* = 7.74, b* = 28.62). For β-carotene, the 73% cassava:27% sample was ~5.2 times more than the level in 100% cassava gari. Also, it had lower residual cyanogenic compounds (0.37 vs. 1.71 mg/kg, p < 0.001, measured as hydrogen cyanide) compared with cassava-only gari. The sensory scores by the 100 panelists using a five-point hedonic scale (1 = dislike extremely to 5 = like extremely) exceeded the minimum threshold (3) for acceptance. Within the limits of this study, OFSP can be composited with cassava up to 27% to process gari that has similar physicochemical properties and sensorial preference as that of cassava only. Furthermore, the OFSP-composited gari contains a significant amount of provitamin A and have a reduced residual cyanogenic compound. Thus, the composited gari could play a significant role in addressing vitamin A deficiency in Ghana compared to the 100% cassava only.