A plasmochemical synthetic strategy for the template-free and one-step preparation of highly crystalline mesoporous TiO 2 from oxidation of titanium tetraisopropoxide (TTIP) aerosol by gliding arc plasma in a vortex air flow within milliseconds is reported. The scanning electron microscopy, high-resolution transmission electron microscopy, and nitrogen sorption characterizations confirm the wormhole-like mesoporous structures. The highly crystalline mesoporous TiO 2 has an optimized anatase/rutile weight ratio of about 80/20 for photocatalytic applications, exhibiting superior thermal stability and good photocatalytic activity.TiO 2 has attracted considerable attentions due to its stability, non-toxicity, and inexpensiveness, and promising photocatalytic applications in degrading pollutants, energy conversion and chemical synthesis. [1] TiO 2 with high specific surface area, large porosity and tunable morphologies is often in demand to achieve the high photocatalytic efficiency. Therefore, mesoporous TiO 2 has aroused increasing interests. [2] For the mesoporous TiO 2 , the preparing techniques are of great concern with its characteristics. The synthesis of mesoporous TiO 2 generally requires soft templates (surfactants and block polymers) and hard templates (e. g., porous silica, polystyrene spheres, porous carbon). [2] Normally, the processes of sol-gel, [2a,3] hydrothermal chemistry, [4] microwave [5] and sonochemistry [6] are widely and employed. However, these synthesis processes inevitably require the costly surfactants and are comparatively complicated and time consuming. [2d] Calcination is the necessary step to remove the template and to obtain crystalline structure. However, the shrinkage of mesoporous structure and agglomeration of the particles will be caused by calcination. [2b,d,7] Recently, the important applications of plasmas for catalyst preparation have been reported increasingly. [8] Herein, we report a plasmochemical synthetic strategy for the templatefree and one-step preparation of highly crystalline mesoporous TiO 2 within milliseconds.In this plasmochemical synthetic strategy, a vortex-flow gliding arc plasma is employed. The plasma features a fast transition from a quasi-thermal stage to a non-thermal stage, providing high electron density (10 13 -10 14 cm À3 ) and gas temperature of over 2000 K in the quasi-thermal stage and high level of non-equilibrium (electron temperature @ gas temperature) in the non-thermal stage. [9] As shown in the left of Figure 1, titanium tetraisopropoxide (TTIP, J&K Scientific, 98%) aerosol as the Ti precursor is generated from an ultrasonic atomizer and carried by 100 mL/min N 2 into the specially designed plasma reactor. The air with a flow rate of 5 L/min enters via two tangential gas inlets of the plasma reactor to generate gliding arc plasma under an input power of 100 W (the middle of Figure 1). The TTIP aerosol is rapidly oxidized by the air plasma and a highly crystalline mesoporous TiO 2 is directly produced (the right of Figure 1), expe...