Developing the lignin-based functional materials for uranium uptake is extremely attractive, but challenging due to the complex structure, poor solubility and reactivity of lignin. Herein, a novel phosphorylated lignin (LP)/sodium alginate/ carboxylated carbon nanotube (CCNT) composite aerogel ([email protected]) with vertically oriented lamellar configuration was created for efficient uranium uptake from acidic wastewater. The successful phosphorylation of lignin by a facile solvent-free mechanochemical method achieved more than six-times enhancement in U(VI) uptake capacity of lignin. While, the incorporation of CCNT not only increased the specific surface area of [email protected], but also improved its mechanical strength as a reinforcing phase. More importantly, the synergies between LP and CCNT components endowed [email protected] with an excellent photothermal performance, resulting in a local heat environment on [email protected] and further boosting the U(VI) uptake. Consequently, the light irradiated [email protected] exhibited an ultrahigh U(VI) uptake capacity (1308.87 mg g−1), 61.26% higher than that under dark condition, excellent adsorptive selectivity and reusability. After exposure to 10 L of simulated wastewater, above 98.21% of U(VI) ions could be rapidly captured by [email protected] under light irradiation, revealing the tremendous feasibility in industrial application. The electrostatic attraction and coordination interaction were considered as the main mechanism for U(VI) uptake.