Biochar from pyrolysis/gasification is relatively poor in oxygen-containing groups and low in micro/mesoporosity, which constrains its adsorption performance. Here, thermal air treatment (TAT) at a mild condition (300 °C in air) was applied to oxygenate the surfaces of various biochars and modify their pore structures for the promotion of their uranium (U(VI)) adsorptions. Results showed that TAT had a high product yield (>76%), increased the O contents, O/C ratios and O-containing groups in biochars, and substantially developed the micro/mesoporosities of biochars. Batch adsorption results showed that TAT remarkably improved U(VI) adsorption capacities of various biochars. Specifically, the maximum U(VI) adsorption capacities of ash-poor corn cob biochar and ash-rich sewage sludge biochar were increased by 137% to 163 mg/g and 23% to 97 mg/g, respectively. Thus, TAT might be a promising strategy to engineer various biochars for adsorptive applications.