TiO 2 with tailored porosity, particle size, and shape in the nanometer range is attracting a lot of attention because of its potential use in photocatalysis and energy conversion. As far as photocatalysis applications are concerned, the use of high surface area TiO 2 as a photocatalyst for pollutant degradation and for water splitting is of particular interest. [1][2][3][4][5][6][7] The presence of bulk defects and grain boundary barriers-associated with the small dimensions of the particles, recombination of electrons, and holes generated by band-gap excitation-is limiting the photoconversion efficiency. [8][9][10] To improve charge separation and the associated catalytic efficiency, researchers have essentially followed two strategies. The first centers on tailoring of the size, shape, and threedimensional organization of TiO 2 particles [1,2,11,12] or of Ti-O-Ti wires with semiconductor character. [5,[13][14][15][16] The second strategy focuses on improving the photocatalytic properties: i) by incorporating metal cations and anions (mainly nitrogen, sulphur, iodine, and other elements) into the bulk; [6,14,[17][18][19][20][21][22][23] ii) by supporting metal particles (mainly Au, Ag, Pt, Ni). [1,3,[24][25][26][27][28][29][30][31] Interesting results are obtained when the two abovementioned research directions are combined to benefit from the sum of their advantages. [32] Several strategies have been adopted for the development of energy conversion applications in solar cells. [1,3,[33][34][35][36] Among them, the use of dye-sensitized TiO 2 nanostructures has an outstanding reputation and both experimental and theoretical evaluations of the efficiency-limiting factors have been identified. [33,37,38] Recently, it has been shown that the use of ordered arrays of TiO 2 nanostructures (either pure, such as nanotubes, nanowires, and nanorods [39][40][41] or TiO 2 -based architectures, [15,42,43] which replace the traditional nanoparticle film) can improve the efficiency. [9,34,40,[43][44][45][46][47][48][49] Moreover, it is evident from recent literature data [1,3,9,44,50] that the innovative synthesis of TiO 2 particle arrays, either pure or anchored to conducting substrates, plays a leading role in both photocatalysis and energy conversion applications.In this paper, we describe a new method for the synthesis of parallelly aligned TiO 2 micropillars, either pure or fixed to a rigid carbon support. Accurate characterization shows that, depending upon the synthesis conditions, the micropillars constitute of partially cemented pure anatase or a mixture of coexisting anatase and rutile particles with a diameter in the 10-20 nm range. The obtained materials combine high surface areas ($60 m 2