The Miao'ershan uranium ore district is one of the most important granite-hosted uranium producers in South China. There are several Triassic granite plutons in the Miao'ershan batholith, but uranium ore deposits mainly occur within the Douzhashan granitic body. Precise zircon U–Pb dating indicated that these Triassic granite plutons were emplaced during 204 to 215Ma. The Douzhashan U-bearing granite lies in the central part of the Miao'ershan batholith, and has higher U contents (8.0 to 26.1ppm, average 17.0ppm) than the nearby Xiangcaoping granite (5.0 to 9.3ppm, average 7.0ppm) and the Yangqiaoling granite (6.4 to 18.3ppm, average 11.5ppm) in the south part of the batholith. The Douzhashan granite is composed of medium-grained two-mica granite, whereas the Xiangcaoping and Yangqiaoling granites are composed of porphyritic biotite granite. Both the Xiangcaoping and Douzhashan granites have high A/CNK ratios (>1.10), high (87Sr/86Sr)i ratios (>0.720) and low εNd(t) values (−11.3 to −10.4), suggesting that they belong to strongly peraluminous S-type granites. The Douzhashan granite has low CaO/Na2O ratios, high Rb/Sr and Rb/Ba ratios, indicating a partial melting origin of clay-rich pelitic rocks. In contrast, the Xiangcaoping granite formed from clay-poor psammite-derived melt. The Yangqiaoling granite shows different geochemical characteristics with the Douzhashan and Xiangcaoping granites, indicating a different magma source. The Yangqiaoling granite has higher εNd(t) of −9.4 to −8.3 and variable A/CNK values from 0.98 to 1.19, suggesting a mixture source of meta-sedimentary rocks and meta-igneous rocks. Crystallization fractionation is not the main mechanism for U enrichment in the Douzhashan granite. We suggest that U-rich pelitic rock sources may be the key factor to generate peraluminous U-bearing granites in South China. Searching for those granites which are reduced, strongly peraluminous and were derived from U-rich pelitic rocks, is the most effective way for exploring granite-hosted U deposits.